4-METHYL-1-PENTENE/alpha-OLEFIN COPOLYMER, COMPOSITION COMPRISING THE COPOLYMER AND 4-METHYL-1-PENTENE COPOLYMER COMPOSITION

ABSTRACT

The present invention provides a 4-methyl-1-pentene/α-olefin copolymer being excellent in lightness, stress absorption, stress relaxation, vibration damping properties, scratch resistance, abrasion resistance, toughness, mechanical properties and flexibility, having no stickiness during molding operation and being excellent in the balance among these properties; a composition comprising the polymer; and uses thereof. The 4-methyl-1-pentene/α-olefin copolymer (A) of the present invention satisfies specific requirements, and comprises 5 to 95 mol % of a structural unit (i) derived from 4-methyl-1-pentene, 5 to 95 mol % of a structural unit (ii) derived from at least one kind of α-olefin selected from α-olefins having 2 to 20 carbon atoms excluding 4-methyl-1-pentene and 0 to 10 mol % of a structural unit (iii) derived from a non-conjugated polyene, provided that the total of the structural units (i), (ii), and (iii) is 100 mol %.

CROSS-REFERENCE TO RELATED APPLICATIONS

The present application is a Continuation of U.S. patent applicationSer. No. 16/848,132, filed on Apr. 14, 2020, which is a Continuation ofU.S. patent application Ser. No. 15/636,542, filed on Jun. 28, 2017(issued as U.S. Pat. No. 10,662,270, on May 26, 2020), which is aDivisional of U.S. patent application Ser. No. 13/505,706, filed on May2, 2012 (issued as U.S. Pat. No. 9,725,540, on Aug. 8, 2017), which is aNational Stage Entry of International Application No. PCT/JP2010/069753,filed on Nov. 5, 2010, which claims the benefit of Japanese PatentApplication No. 2009-255071, filed on Nov. 6, 2009, and Japanese PatentApplication No. 2010-003166, filed on Jan. 8, 2010. The entire contentsof which are hereby incorporated by reference in their entireties.

TECHNICAL FIELD

The present invention relates to a 4-methyl-1-pentene/α-olefincopolymer, a composition comprising the copolymer, an article comprisingthe composition, and uses thereof.

In more detail, the present invention relates to a copolymer of4-methyl-1-pentene and an α-olefin, the copolymer being excellent inflexibility, lightness, stress absorption, stress relaxation, scratchresistance, abrasion resistance, toughness, and mechanical properties,having no stickiness in molding operation and being excellent in thebalance among these properties; and the present invention furtherrelates to a composition comprising the copolymer and uses thereof.

BACKGROUND ART

Olefin polymers, being excellent in processability, chemical resistance,electrical properties, mechanical properties, and the like, areprocessed to extrusion molded articles, injection molded articles,hollow articles, films, sheets, fibers, and the like, and are used inmany applications including daily goods, kitchenware, packaging films,nonwoven fabrics, household electrical appliances, mechanical parts,electrical parts, and automotive parts.

In particular, olefin polymers comprising 4-methyl-1-pentene are used invarious fields including food, medical treatment, electronicinformation, household electrical appliances, experimental equipment andstationery, as a resin being excellent in lightness, transparency, gaspermeability, chemical resistance, and furthermore heat resistance.

These olefin polymers are generally produced using a catalyst comprisinga transition metal compound and an organoaluminum compound, i.e.,so-called Ziegler catalyst.

Patent Document 1 proposes a 4-methyl-1-pentene random copolymer, and acomposition containing the copolymer.

However, the copolymer in this document has multiple reaction sites,thus having a drawback of involving the easy generation of a lowstereoregularity polymer or a low-molecular weight polymer. Thesepolymers cause an adverse influence as a sticky component during filmformation. Further, the copolymer in this document involves thebleeding-out of the low-molecular weight component to the surface, andhas decreased mechanical properties such as toughness and strength. Theimprovement as a product is thus needed.

On the other hand, olefin polymers obtained using an organometalliccomplex catalyst containing a cyclopentadienyl group are generallycharacterized by the polymers having a uniform composition in terms ofe.g., the molecular weight, but it is pointed out that these polymersare inferior in heat resistance as compared with polymers obtained usingconventional Ziegler catalysts. The reason is said to be attributable tothe heterogeneous bond of monomer units contained in several percentagein the olefin polymers produced using usual metallocene catalysts,resulting in adverse influence in physical properties.

Patent Document 2 proposes a 4-methyl-1-pentene polymer having excellentheat resistance and a high molecular weight with a narrow molecularweight distribution. However, the polymers obtained therein still needto be improved in terms of heat resistance, toughness, and moldingprocessability.

Poly(4-methyl-1-pentene) is excellent in releasability.Poly(4-methyl-1-pentene), because of its lower surface tension ascompared with other resins, exhibits excellent releasability duringmolding operation, i.e., poor compatibility with other resins. As aresult, the use of other resins as a modifier to modifypoly(4-methyl-1-pentene) in terms of e.g., toughness, impact propertiesresults in the failure to exhibit these properties. Patent Document 3and Patent Document 4 deal with this problem by proposing the use of4-methyl-1-pentene polymer compositions. However, these compositionsneed to be further improved in terms of toughness, impact resistance,and transparency.

Meanwhile, vibration dampers are widely used to prevent or dampenvibration caused by device components and then reduce the vibration toan appropriate level. The vibration dampers are used also as a materialhaving specific vibration damping properties to provide a high qualitysound in a speaker and the like of audio devices.

As a polymer material having vibration damping properties, conventionalart provides a material having a large peak value of loss coefficienttan δ, as obtained by measuring a dynamic viscoelasticity thereof, theloss tangent tan δ being an indicator of vibration damping properties ofthe polymer material. Examples of the material includestyrene/isoprene/styrene block copolymer (SIS) and hydrogenated productsthereof.

SIS, having a large peak of loss tangent tan δ at around a roomtemperature, has excellent vibration damping properties at around a roomtemperature. However, SIS, because of having a sharp peak of tan δ, hasinferior vibration damping properties at a temperature that is notaround a room temperature. Meanwhile, the hydrogenated SIS, which isproduced through a two-stage process of polymerization andhydrogenation, costs high for its production; and thus, an industrialapplication thereof is limited.

A rubber vibration damper has excellent properties in its performance,but is difficult to form so as to have an arbitrary shape in itspractical use. Polypropylene and 4-methyl-1-pentene homopolymer havetheir tan δ peaks at around a room temperature. The peak values,however, are small, and this leads to a problem such as low sizeprecision during molding operation. A polyvinyl chloride (PVC) vibrationdamper possibly has an adverse influence on environment by, e.g.,emitting harmful gas during burning.

For these reasons, there has been desired a material excellent inlightness, flexibility, stress absorption, stress relaxation, vibrationdamping properties, toughness, scratch resistance, abrasion resistance,and mechanical properties, having no stickiness during molding operationand being excellent in the balance among these properties.

CITATION LIST Patent Documents

Patent Document 1: JP-A-2008-144155

Patent Document 2: WO 2005/121192

Patent Document 3: WO 1996/28507

Patent Document 4: WO 2002/081958

SUMMARY OF THE INVENTION Problems to be Solved by the Invention

The present invention is intended to solve the problems as describedabove, and it is an object of the invention to provide a4-methyl-1-pentene/α-olefin copolymer being excellent in lightness,flexibility, stress absorption, stress relaxation, vibration dampingproperties, scratch resistance, abrasion resistance, toughness, andmechanical properties, having no stickiness during molding operation andbeing excellent in the balance among these properties. It is anotherobject of the invention to provide a composition comprising thecopolymer, and an article comprising the composition.

Means to Solve the Problems

The present inventors earnestly studied and then, completed the presentinvention.

Namely, a 4-methyl-1-pentene/α-olefin copolymer (A) of the presentinvention comprises:

5 to 95 mol % of a structural unit (i) derived from 4-methyl-1-pentene,

5 to 95 mol % of a structural unit (ii) derived from at least one kindof α-olefin selected from α-olefins having 2 to 20 carbon atomsexcluding 4-methyl-1-pentene, and

0 to 10 mol % of a structural unit (iii) derived from a non-conjugatedpolyene, provided that the total of the structural units (i), (ii), and(iii) is 100 mol %; and

satisfies the following requirements (a) to (d).

(a) the intrinsic viscosity [η], as measured in a decalin at 135° C., is0.01 to 5.0 dL/g,

(b) the ratio (Mw/Mn) of a weight-average molecular weight (Mw) to anumber-average molecular weight (Mn), as measured by gel permeationchromatography (GPC), is 1.0 to 3.5,

(c): the tensile modulus (YM) is 0.1 to 1000 MPa, and

(d): the melting point [Tm], as measured by differential scanningcalorimetry (DSC), is lower than 110° C. or not observed.

In terms of flexibility, mechanical properties, toughness, scratchresistance, abrasion resistance, and stress absorption, it is preferablethat the copolymer comprises 10 to 90 mol % of the structural unit (i)and 10 to 90 mol % of the structural unit (ii), provided that the totalof the structural units (i) and (ii) is 100 mol %, and further satisfiesthe following requirements (c1) and (e).

(c1): The tensile modulus (YM) is 0.1 to 300 MPa.

(e): The difference ΔHS in Shore A hardness between immediately afterthe starting of indenter contact and 15 seconds after the starting ofindenter contact is 10 to 50 (Shore A hardness is measured using a presssheet thereof having a thickness of 3 mm in accordance with JIS K6253).With regard to a method for measuring Shore A hardness, Examples can bereferred to (the same is applied hereinafter).

A 4-methyl-1-pentene/α-olefin copolymer (A3) comprises:

5 to 95 mol % of the structural unit (i),

4.9 to 94.9 mol % of the structural unit (ii), and

0.1 to 10 mol % of the structural unit (iii), provided that the total ofthe structural units (i), (ii), and (iii) is 100 mol %.

The 4-methyl-1-pentene/α-olefin copolymer (A3) is more preferable interms of mechanical properties, flexibility, and toughness.

A 4-methyl-1-pentene/α-olefin copolymer (A1) comprises: 5 to 50 mol %,preferably 10 to 32 mol % of the structural unit (i),

50 to 95 mol %, preferably 68 to 90 mol % of the structural unit (ii),and

0 to 10 mol % of the structural unit (iii), provided that the total ofthe structural units (i), (ii), and (iii) is 100 mol %, and

satisfies the following requirement (j), in addition to the requirements(a) to (d).

(j): The maximum value of loss tangent tan δ, as obtained by measuring adynamic viscoelasticity thereof within a temperature range of −70 to180° C. at a frequency of 10 rad/s, is within a temperature range of 0to 40° C. and the maximum value of tan δ is 0.5 or more.

In terms of stress absorption, stress relaxation, and flexibility, it ispreferable that the copolymer (A1) comprises 10 to 32 mol % of thestructural unit (i), 68 to 90 mol % of the structural unit (ii), and 0to 10 mol % of the structural unit (iii), provided that the total of thestructural units (i), (ii), and (iii) is 100 mol %.

A 4-methyl-1-pentene/α-olefin copolymer (A2) comprises:

33 to 80 mol % of the structural unit (i),

67 to 20 mol % of the structural unit (ii), and

0 to 10 mol % of the structural unit (iii), provided that the total ofthe structural units (i), (ii), and (iii) is 100 mol %, and

satisfies the following requirement (e1), in addition to therequirements (a) to (d).

(e1) The difference ΔHS in Shore A hardness between immediately afterthe starting of indenter contact and 15 seconds after the starting ofindenter contact is 15 to 50.

A 4-methyl-1-pentene/α-olefin copolymer composition (X) of the presentinvention comprises:

5 to 95 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer,and

5 to 95 parts by weight of a thermoplastic resin (B) other than the4-methyl-1-pentene/α-olefin copolymer, provided that the total of thecopolymer and the thermoplastic resin (B) is 100 parts by weight.

In terms of heat resistance, mechanical properties, toughness, andabrasion resistance, it is preferable that the composition (X) comprises5 to 49 parts by weight of the copolymer and 95 to 51 parts by weight ofa crystalline olefin resin (B1) other than the4-methyl-1-pentene/α-olefin copolymer as the thermoplastic resin (B),provided that the total of the copolymer and (B1) is 100 parts by weight(X12 and X22).

In terms of flexibility, stress absorption, stress relaxation, andmechanical properties, it is preferable that the composition (X)comprises 50 to 95 parts by weight of the copolymer (A) and 5 to 50parts by weight of the crystalline olefin resin (B1), provided that thetotal of (A) and (B) is 100 parts by weight (X11 and X21).

The 4-methyl-1-pentene/α-olefin copolymer composition (X11) comprises:

50 to 95 parts by weight of a 4-methyl-1-pentene/α-olefin copolymercomprising 10 to 32 mol % of the structural unit (i), 68 to 90 mol % ofthe structural unit (ii), and 0 to 10 mol % of the structural unit(iii), provided that the total of the structural units (i), (ii), and(iii) is 100 mol %, and satisfying at least the requirements (a) to (d),and

5 to 50 parts by weight of a thermoplastic resin (B) other than the4-methyl-1-pentene/α-olefin copolymer, provided that the total of thecopolymer (A) and the thermoplastic resin (B) is 100 parts by weight);and

satisfies the following requirement (j1).

(j1): The maximum value of loss tangent tan δ, as obtained by measuringa dynamic viscoelasticity thereof within a temperature range of −70 to180° C. at a frequency of 10 rad/s, is within a temperature range of −50to 40° C. and the maximum value of tan δ is 0.4 or more.

The 4-methyl-1-pentene/α-olefin copolymer composition (X12) comprises:

5 to 49 parts by weight of a 4-methyl-1-pentene/α-olefin copolymercomprising 10 to 32 mol % of the structural unit (i), 68 to 90 mol % ofthe structural unit (ii), and 0 to 10 mol % of the structural unit(iii), provided that the total of the structural units (i), (ii), and(iii) is 100 mol %, and satisfying at least the requirements (a) to (d),and

51 to 95 parts by weight of a thermoplastic resin (B) other than the4-methyl-1-pentene/α-olefin copolymer, provided that the total of thecopolymer (A) and the thermoplastic resin (B) is 100 parts by weight.

In terms of providing heat resistance, mechanical properties, andtoughness, it is preferable that the copolymer composition (X12)comprises the thermoplastic resin (B) being at least one crystallineolefin resin (B1) selected from polypropylene, poly(4-methyl-1-pentene),polyethylene, and polybutene, and satisfies the following requirements(f) and (g).

(f): The softening temperature is 110 to 250° C.

(g): The tensile modulus (YM) is 300 to 2000 MPa.

The 4-methyl-1-pentene/α-olefin copolymer composition (X21) comprises:

50 to 95 parts by weight of a 4-methyl-1-pentene/α-olefin copolymercomprising 33 to 80 mol % of the structural unit (i), 67 to 20 mol % ofthe structural unit (ii) and 0 to 10 mol % of the structural unit (iii),provided that the total of the structural units (i), (ii), and (iii) is100 mol %, and satisfying at least the requirements (a) to (d), and

5 to 50 parts by weight of a thermoplastic resin (B) other than the4-methyl-1-pentene/α-olefin copolymer, provided that the total of thecopolymer (A) and the thermoplastic resin (B) is 100 parts by weight;and

satisfies the following requirement (e2).

(e2): The difference ΔHS in Shore A hardness between immediately afterthe starting of indenter contact and 15 seconds after the starting ofindenter contact is 10 to 50, or

the difference ΔHS in Shore D hardness between immediately after thestarting of indenter contact and 15 seconds after the starting ofindenter contact is 5 to 50.

In terms of flexibility, stress relaxation, and mechanical properties,it is preferable that the copolymer composition (X21) comprises 50 to 95parts by weight of the copolymer and 5 to 50 parts by weight of thecrystalline olefin resin (B1), provided that the total of the copolymerand (B1) is 100 parts by weight.

The 4-methyl-1-pentene/α-olefin copolymer composition (X22) comprises:

5 to 49 parts by weight of a 4-methyl-1-pentene/α-olefin copolymercomprising 33 to 80 mol % of the structural unit (i), 67 to 20 mol % ofthe structural unit (ii) and 0 to 10 mol % of the structural unit (iii),provided that the total of the structural units (i), (ii), and (iii) is100 mol %, and satisfying at least the requirements (a) to (d), and

51 to 95 parts by weight of a thermoplastic resin (B) other than the4-methyl-1-pentene/α-olefin copolymer, provided that the total of thecopolymer (A) and the thermoplastic resin (B) is 100 parts by weight.

In terms of heat resistance, mechanical properties, abrasion resistance,and toughness, it is preferable that the composition (X22) comprises 5to 49 parts by weight of the copolymer and 95 to 51 parts by weight of acrystalline olefin resin (B1) other than the 4-methyl-1-pentene/α-olefincopolymer as the thermoplastic resin (B), provided that the total of thecopolymer and (B1) is 100 parts by weight.

In terms of heat resistance, mechanical properties, and toughness, it ispreferable that the copolymer composition (X22) comprises thethermoplastic resin (B) being at least one crystalline olefin resin (B1)selected from polypropylene, poly(4-methyl-1-pentene), polyethylene, andpolybutene, and satisfies the following requirements (f) and (g).

(f): The softening temperature is 110 to 250° C., preferably 120 to 240°C.

(g): The tensile modulus (YM) is 300 to 2000 MPa, preferably 400 to 2000MPa.

A4-methyl-1-pentene copolymer composition (Y) of the present inventioncomprises:

50 to 98 parts by weight of a 4-methyl-1-pentene copolymer (AA),

1 to 49 parts by weight of a crystalline olefin resin (BB) having amelting point of 100° C. or higher other than the 4-methyl-1-pentenecopolymer (AA), and

1 to 49 parts by weight of an α-olefin copolymer (CC) having a meltingpoint of lower than 100° C. other than the 4-methyl-1-pentene copolymer(AA), provided that the total of (AA), (BB), and (CC) is 100 parts byweight,

wherein the copolymer (AA) satisfies the following requirements (a-1) to(a-3), (b-2) and (b-3), and preferably (b-1).

In terms of improvement in mechanical properties, stress absorption, andvibration damping properties, the copolymer composition (Y) satisfyingthe requirements (a-1) to (a-3), and (b-2) to (b-3) is preferable.

(a-1): The copolymer (AA) comprises 5 to 95 wt % of a structural unitderived from 4-methyl-1-pentene and 5 to 95 wt % of a structural unitderived from at least one kind of α-olefin selected from α-olefinshaving 2 to 20 carbon atoms excluding 4-methyl-1-pentene, provided thatthe total of the structural units in the copolymer (AA) is 100 wt %.

(a-2): The intrinsic viscosity [η], as measured in a decalin at 135° C.,is 0.01 to 5.0 dL/g.

(a-3): The ratio (Mw/Mn) of a weight-average molecular weight (Mw) to anumber-average molecular weight (Mn), as measured by gel permeationchromatography (GPC), is 1.0 to 3.5.

(b-1): The copolymer (AA) comprises 10 to 90 wt % of a structural unitderived from 4-methyl-1-pentene and 10 to 90 wt % of a structural unitderived from at least one kind of α-olefin selected from α-olefinshaving 2 to 20 carbon atoms excluding 4-methyl-1-pentene, provided thatthe total of the structural units in the copolymer (AA) is 100 wt %.

(b-2): The difference ΔHS in Shore A hardness between immediately afterthe starting of indenter contact and 15 seconds after the starting ofindenter contact is 10 to 50.

(b-3): The melting point [Tm], as measured by differential scanningcalorimetry (DSC), is lower than 110° C. or not observed.

In terms of improvement in mechanical properties, stress absorption, andvibration damping properties, it is preferable that the composition (Y)comprises:

50 to 96 parts by weight, preferably 50 to 90 parts by weight of thecopolymer (AA),

2 to 45 parts by weight, preferably 5 to 45 parts by weight of the resin(BB), and

2 to 45 parts by weight, preferably 5 to 45 parts by weight of theα-olefin copolymer (CC), and that the copolymer (AA) satisfies thefollowing requirement (c-1).

(c-1): The copolymer (AA) comprises:

18 to 90 wt %, preferably 25 to 85 wt % of a structural unit derivedfrom 4-methyl-1-pentene, and

10 to 82 wt %, preferably 15 to 75 wt % of a structural unit derivedfrom at least one kind of α-olefin selected from α-olefins having 2 to20 carbon atoms excluding 4-methyl-1-pentene, provided that the total ofthe structural units in the copolymer (AA) is 100 wt %.

It is preferable that the copolymer composition (Y) has a difference ΔHSin Shore A hardness between immediately after the starting of indentercontact and 15 seconds after the starting of indenter contact being 10to 50; or has a difference ΔHS in Shore D hardness between immediatelyafter the starting of indenter contact and 15 seconds after the startingof indenter contact being 5 to 50.

In terms of mechanical properties, it is preferable that the copolymercomposition (Y) comprises the crystalline olefin resin (BB) being atleast one kind selected from polypropylene, poly(4-methyl-1-pentene),polyethylene, and polybutene. It is more preferable that the crystallineolefin resin (B) is polypropylene in terms of mechanical properties.

In terms of mechanical properties, it is preferable that the copolymercomposition (Y) comprises the α-olefin copolymer (CC) satisfying thefollowing requirements (d-1) and (d-2).

(d-1): The α-olefin copolymer (CC) comprises 50 to 99 wt % of astructural unit derived from ethylene, propylene or butene-1 and 1 to 50wt % of a structural unit derived from an α-olefin having 2 to 20 carbonatoms other than the above-mentioned structural unit, provided that thetotal of the structural units in the copolymer (CC) is 100 wt %.

(d-2): MFR, as measured at 190° C. or 230° C. under a load of 2.16 kg inaccordance with JIS K-6721, is in the range of 0.01 to 100 g/10 minutes,and the density is in the range of 0.910 to 0.850 g/cm³.

An article of the present invention comprises any one or more of the4-methyl-1-pentene/α-olefin copolymer, the 4-methyl-1-pentene/α-olefincopolymer composition, and the 4-methyl-1-pentene copolymer composition.

Effect of the Invention

The 4-methyl-1-pentene/α-olefin copolymer and the composition comprisingthe copolymer according to the present invention, and the article of thepresent invention are excellent in lightness, flexibility, stressabsorption, stress relaxation, vibration damping properties, scratchresistance, abrasion resistance, toughness, transparency, mechanicalproperties, moldability, and releasability, and have no stickinessduring molding operation and are excellent in the balance among theseproperties.

EMBODIMENTS FOR CARRYING OUT THE INVENTION

The present invention is described specifically hereinafter.

4-Methyl-1-pentene/α-olefin copolymers (A), and (A1) to (A3)

The 4-methyl-1-pentene/α-olefin copolymer (A) according to the presentinvention comprises:

5 to 95 mol % of a structural unit (i) derived from 4-methyl-1-pentene,

95 to 5 mol % of a structural unit (ii) derived from at least one kindof α-olefin selected from α-olefins having 2 to 20 carbon atomsexcluding 4-methyl-1-pentene, and

0 to 10 mol % of a structural unit (iii) derived from a non-conjugatedpolyene, provided that the total of the structural units (i), (ii), and(iii) is 100 mol %.

This copolymer comprises the structural unit (i) preferably in an amountof 10 to 90 mol %, more preferably 15 to 85 mol %, still more preferably15 to 80 mol %, most preferably 15 to 75 mol %; and the structural unit(ii) preferably in an amount of 90 to 10 mol %, more preferably 85 to 15mol %, still more preferably 85 to 20 mol %, most preferably 85 to 25mol %, provided that the total of the structural units (i) and (ii) is100 mol %. In the present invention, “an α-olefin having 2 to 20 carbonatoms” does not include 4-methyl-1-pentene, unless otherwise noted.

Meanwhile, any other copolymerization component may be containedtherein, to the degree not adversely affecting the object of the presentinvention; and the embodiments thereof are within a scope of the presentinvention.

In addition, the copolymer (A) satisfies at least the followingrequirements (a) to (d).

(a): The copolymer (A) has an intrinsic viscosity [η] in decalin at 135°C. in the range of 0.01 to 5.0 (dL/g), preferably 0.05 to 4.0 (dL/g),more preferably 0.1 to 3.0 (dL/g), still more preferably 0.5 to 2.5(dL/g). The use of a catalyst described later can provide the polymerwithout impairing the molecular weight distribution. The combined use ofhydrogen during polymerization, as described later, can control amolecular weight of the polymer and provide polymers having molecularweights ranging from low to high without limitation.

(b): The copolymer (A) has a ratio (Mw/Mn) of a weight-average molecularweight (Mw) to a number-average molecular weight (Mn), as measured bygel permeation chromatography (GPC), in the range of 1.0 to 3.5,preferably 1.5 to 3.0, more preferably 1.5 to 2.5. A large Mw/Mn,raising a concern in terms of the influence of a compositiondistribution and a low-molecular weight polymer, may prevent the polymerfrom exhibiting mechanical properties, moldability, and abrasionresistance, and cause the polymer to have stickiness during moldingoperation. The Mw/Mn in the range from 1.0 to 3.5 is advantageous inexhibiting the foregoing characteristics and thus is of a highindustrial value. The use of a catalyst described later can provide thepolymer having a Mw/Mn within the above range without impairing themolecular weight. If an application requires the4-methyl-1-pentene/α-olefin copolymer to have a wide molecular weightdistribution, this need can be satisfied by blending polymers differingin molecular weight, or by employing a multistep polymerization method,or the like.

With regard to the copolymer (A), the extracted amount thereof undermethyl acetate is 0 to 1.5 wt %, preferably 0 to 1.0 wt %, morepreferably 0 to 0.8 wt %, most preferably 0 to 0.6 wt %. The extractedamount under methyl acetate is an indicator of stickiness during moldingoperation. If this value is large, the resultant polymer has a largecomposition distribution thereby containing a low-molecular weightpolymer, which causes the problem during molding operation. Theextracted amount under methyl acetate being within the above rangecauses no problem due to stickiness during molding operation.

The copolymer (A) has a weight-average molecular weight (Mw) in terms ofpolystyrene, as measured by gel permeation chromatography (GPC),preferably in the range of 500 to 10,000, 000, more preferably 1,000 to5,000,000, still more preferably 1,000 to 2,500,000.

The copolymer (A) has a parameter B value, as measured by ¹³C-NMR, whichshows randomness of a chain distribution of the copolymerized monomers,preferably in a range of 0.9 to 1.5, more preferably 0.9 to 1.3, stillmore preferably 0.9 to 1.2. When the parameter B value is within theabove range, the polymer has good randomness of chain distribution ofmonomers, has no composition distribution, and is excellent in e.g.,transparency, flexibility, stress absorption and stress relaxation.

(c): The copolymer (A) has a tensile modulus (YM) of 0.1 to 1000 MPa,preferably 0.1 to 500 MPa, more preferably 0.1 to 300 MPa, still morepreferably 0.1 to 200 MPa. When the tensile modulus is within the aboverange, for example, mechanical properties, toughness, flexibility, andstress absorption are excellent.

(d): The copolymer (A) has a melting point (Tm), as measured by DSC, ofpreferably lower than 110° C. or not observed, more preferably lowerthan 100° C. or not observed, still more preferably lower than 85° C. ornot observed. The melting point of the copolymer (A) can be variedarbitrarily by types and compositions of the comonomers. When themelting point is within the above range, flexibility and toughness areexcellent.

The copolymer (A) has a density, as measured in accordance with ASTMD1505 (water replacement method), preferably in the range of 0.810 to0.850 g/cm³, more preferably 0.820 to 0.850 g/cm³, more preferably 0.830to 0.850 g/cm³.

It is preferable that the copolymer (A) satisfies the followingrequirements (c1) and (e).

(c1): The tensile modulus (YM) is 0.1 to 300 MPa, preferably 0.1 to 250MPa, more preferably 0.3 to 200 MPa. When the tensile modulus is withinthe above range, mechanical properties, toughness, flexibility, andstress absorption are excellent.

(e): The change ΔHS in Shore A hardness between immediately after themeasurement and 15 seconds after the measurement is 10 to 50, preferably15 to 50, more preferably 20 to 50. The change in Shore A hardness isobtained as follows in accordance with JIS K 6253.

ΔHS=(Shore A hardness 15 seconds after the measurement−Shore A hardnessimmediately after the measurement)

The ΔHS value can be varied arbitrarily by types and compositions ofcomonomers. When ΔHS is within the above range, stress absorption andstress relaxation are excellent.

A 4-methyl-1-pentene/α-olefin copolymer (A1) comprises:

5 to 50 mol %, preferably 10 to 32 mol % of a structural unit (i)derived from 4-methyl-1-pentene,

50 to 95 mol %, preferably 68 to 90 mol % of a structural unit (ii)derived from at least one kind of α-olefin selected from α-olefinshaving 2 to 20 carbon atoms excluding 4-methyl-1-pentene, and

0 to 10 mol %, preferably 0 to 5 mol % of a structural unit (iii)derived from a non-conjugated polyene, provided that the total of thestructural units (i), (ii), and (iii) is 100 mol %, and

satisfies the following requirement (j), in addition to at least therequirements (a) to (d).

The 4-methyl-1-pentene/α-olefin copolymer (A1) is preferable because ofhaving excellent stress absorption and flexibility.

(j): The maximum value of loss tangent tan δ, as obtained by measuring adynamic viscoelasticity thereof within a temperature range of −70 to180° C. at a frequency of 10 rad/s, is within a temperature range of 0to 40° C., and the maximum value of tan δ is 0.5 or more, preferably 0.7or more, more preferably 1.0 or more, most preferably 1.5 or more. Theabove ranges are preferable because the copolymer has excellent stressabsorption.

In terms of providing excellent stress absorption and flexibility, it ispreferable that the copolymer (A1) comprises:

5 to 50 mol %, preferably 5 to 48 mol % of the structural unit (i),

49.9 to 94.9 mol %, preferably 47.9 to 94.9 mol % of the structural unit(ii), and

0.1 to 10 mol %, preferably 0.1 to 5 mol %, more preferably 0.1 to 4.1mol % of the structural unit (iii), provided that the total of thestructural units (i), (ii), and (iii) is 100 mol %, and

satisfies the following requirement (jj), in addition to at least therequirements (a) to (d).

(jj): The maximum value of loss tangent tan δ, as obtained by measuringa dynamic viscoelasticity thereof within a temperature range of −70 to180° C. at a frequency of 10 rad/s, is within a temperature range of −50to 40° C., and the maximum value of tan δ is 0.5 or more, preferably 1.0or more, more preferably 1.5 or more, most preferably 2.0 or more. Theabove ranges are preferable because the copolymer has excellent stressabsorption.

The copolymer (A1) has a ball drop resilience ratio, as obtained bydropping a rigid ball of 16.310 g from a height of 460 mm under a roomtemperature of 25° C. in accordance with JIS K6400, of 0 to 25%,preferably 0 to 20%, more preferably 0 to 15%. The above ranges arefurther preferable in terms of stress absorption.

The copolymer (A1) comprises, in terms of wt % instead of mol %,

10 to 67 wt %, preferably 18 to 49 wt % of a structural unit (i) derivedfrom 4-methyl-1-pentene,

33 to 90 wt %, preferably 51 to 82 wt % of a structural unit (ii)derived from at least one kind of α-olefin selected from α-olefinshaving 2 to 20 carbon atoms excluding 4-methyl-1-pentene, and

0 to 23 wt % of a structural unit (iii) derived from a non-conjugatedpolyene, provided that the total of the structural units (i), (ii), and(iii) is 100 wt %.

A 4-methyl-1-pentene/α-olefin copolymer (A2) comprises:

33 to 80 mol %, preferably 50 to 75 mol % of the structural unit (i),

67 to 20 mol %, preferably 50 to 25 mol % of the structural unit (ii),and

0 to 10 mol %, preferably 0 to 5 mol % of the structural unit (iii),provided that the total of the structural units (i), (ii), and (iii) is100 mol %; and

satisfies any one or more of Shore A hardness and Shore D hardness inthe following requirement (e1), in addition to at least the requirements(a) to (d).

The 4-methyl-1-pentene/α-olefin copolymer (A2) is preferable because ofhaving excellent stress relaxation.

(e1): The difference ΔHS in Shore A hardness between immediately afterthe starting of indenter contact and 15 seconds after the starting ofindenter contact is 15 to 50, preferably 20 to 50, more preferably 23 to50; or

the difference ΔHS in Shore D hardness between immediately after thestarting of indenter contact and 15 seconds after the starting ofindenter contact is 5 to 50, preferably 8 to 50, more preferably 10 to50.

Further, in terms of stress relaxation and abrasion resistance, it ispreferable that the copolymer (A2) has a percentage of change in gloss,as measured by abrasion using Gakushin-type rubbing tester, of 0 to 13,preferably 0 to 10.

A 4-methyl-1-pentene/α-olefin copolymer (A3) of the present inventionsatisfies at least the requirements (a) to (d) and comprises 5 to 95 mol% of the structural unit (i), 94.9 to 4.9 mol % of the structural unit(ii), and 0.1 to 10 mol % of the structural unit (iii), provided thatthe total of the structural units (i), (ii), and (iii) is 100 mol %.

The 4-methyl-1-pentene/α-olefin copolymer (A3) comprises: the structuralunit (i) preferably in an amount of 10 to 90 mol %, more preferably 15to 85 mol %, still more preferably 15 to 70 mol %,

the structural unit (ii) preferably in an amount of 89.9 to 2 mol %,more preferably 84.7 to 8 mol %, still more preferably 84.5 to 25 mol %,and

the structural unit derived from a non-conjugated polyene (iii)preferably in an amount of 0.1 to 8 mol %, more preferably 0.3 to 7 mol%, still more preferably 0.5 to 5 mol %, provided that the total of thestructural units (i), (ii), and (iii) is 100 mol %.

The melting point (d) of the 4-methyl-1-pentene/α-olefin copolymer (A3)can be varied arbitrarily by types and compositions of the comonomers.When the melting point is within the above range, flexibility andtoughness are excellent.

In the present invention, examples of the α-olefin having 2 to 20 carbonatoms used in the 4-methyl-1-pentene/α-olefin copolymer include linearor branched α-olefins, cyclic olefins, aromatic vinyl compounds,conjugated dienes, and functionalized vinyl compounds, excluding4-methyl-1-pentene. The α-olefin in the 4-methyl-1-pentene/α-olefincopolymer of the present invention does not include a non-conjugatedpolyene.

The linear α-olefins are those having 2 to 20 carbon atoms, preferably 2to 15 carbon atoms, more preferably 2 to 10 carbon atoms, with examplesthereof including ethylene, propylene, 1-butene, 1-pentene, 1-hexene,1-octene, 1-decene, 1-undecene, 1-dodecene, 1-tetradecene, 1-hexadecene,1-octadecene, and 1-eicosene; and ethylene, propylene, 1-butene,1-pentene, 1-hexene, and 1-octene are preferable.

The branched α-olefins are those preferably having 5 to 20 carbon atoms,more preferably 5 to 15 carbon atoms, with examples thereof including3-methyl-1-butene, 3-methyl-1-pentene, 3-ethyl-1-pentene,4,4-dimethyl-1-pentene, 4-methyl-1-hexene, 4,4-dimethyl-1-hexene,4-ethyl-1-hexene, and 3-ethyl-1-hexene.

The cyclic olefins are those preferably having 3 to 20 carbon atoms,more preferably 5 to 15 carbon atoms, with examples thereof includingcyclopentene, cyclohexene, cycloheptene, norbornene,5-methyl-2-norbornene, tetracyclododecene, and vinyl cyclohexane.

Examples of the aromatic vinyl compound include styrene, and a mono- ora poly-alkyl styrene such as α-methyl styrene, o-methyl styrene,m-methyl styrene, p-methyl styrene, o,p-dimethylstyrene, o-ethylstyrene, m-ethyl styrene, and p-ethyl styrene.

The conjugated dienes are those having 4 to 20 carbon atoms, preferably4 to 10 carbon atoms, with examples thereof including 1,3-butadiene,isoprene, chloroprene, 1,3-pentadiene, 2,3-dimethyl butadiene,4-methyl-1,3-pentadiene, 1,3-hexadiene, and 1,3-octadiene.

Example of the functionalized vinyl compounds include hydroxylgroup-containing olefins; halogenated olefins; unsaturated carboxylicacids such as (meth)acrylic acid, propionic acid, 3-butenoic acid,4-pentenoic acid, 5-hexenoic acid, 6-heptenoic acid, 7-octenoic acid,8-nonenoic acid, 9-decenoic acid, and 10-undecenoic acid; unsaturatedamines such as allylamine, 5-hexeneamine, and 6-hepteneamine;(2,7-octadienyl) succinic anhydride, pentapropenyl succinic anhydride,unsaturated carboxylic acid anhydrides such as those obtained from theafore-mentioned unsaturated carboxylic acids; unsaturated carboxylichalides such as halogenated compounds obtained from the afore-mentionedunsaturated carboxylic acids; unsaturated epoxy compounds such as4-epoxy-1-butene, 5-epoxy-1-pentene, 6-epoxy-1-hexene,7-epoxy-1-heptene, 8-epoxy-1-octene, 9-epoxy-1-nonene,10-epoxy-1-decene, and 11-epoxy-1-undecene; and ethylenic unsaturatedsilane compounds such as vinyl triethoxy silane, vinyl trimethoxysilane,3-acryloxypropyltrimethoxysilane, γ-glycidoxypropyltripyl trimethoxysilane, y-aminopropyl triethoxysilane, and y-methacryloxypropyltrimethoxy silane.

The hydroxyl group-containing olefins are not particularly limited, aslong as being hydroxyl group-containing olefin compounds, with examplesthereof including hydroxyl group-terminated olefin compounds. Examplesof the hydroxyl group-terminated olefin compounds include:

linear hydroxylated α-olefins having 2 to 20, preferably 2 to 15 carbonatoms, such as vinyl alcohols, allyl alcohols, hydroxylated 1-butene,hydroxylated 1-pentene, hydroxylated 1-hexene, hydroxylated 1-octene,hydroxylated 1-decene, hydroxylated 1-undecene, hydroxylated 1-dodecene,hydroxylated 1-tetradecene, hydroxylated 1-hexadecene, hydroxylated1-octadecene, and hydroxylated 1-eicosene; and

branched hydroxylated α-olefins having 5 to 20 carbon atoms, preferably5 to 15 carbon atoms, such as hydroxylated 3-methyl-1-butene,hydroxylated 3-methyl-1-pentene, hydroxylated 4-methyl-1-pentene,hydroxylated 3-ethyl-1-pentene, hydroxylated 4,4-dimethyl-1-pentene,hydroxylated 4-methyl-1-hexene, hydroxylated 4,4-dimethyl-1-hexene,hydroxylated 4-ethyl-1-hexene, and hydroxylated 3-ethyl-1-hexene.

The halogenated olefins are halogenated α-olefins having an atombelonging to Group 17 of the periodic table, such as chlorine, bromine,and iodine, with examples thereof including:

linear halogenated α-olefins having 2 to 20 carbon atoms, preferably 2to 15 carbon atoms, such as a halogenated vinyl, a halogenated 1-butene,a halogenated 1-pentene, a halogenated 1-hexene, a halogenated 1-octene,a halogenated 1-decene, a halogenated 1-dodecene, a halogenated1-undecene, a halogenated 1-tetradecene, a halogenated 1-hexadecene, ahalogenated 1-octadecene, and a halogenated 1-eicosene; and

branched halogenated α-olefins having 5 to 20 carbon atoms, preferably 5to 15 carbon atoms, such as a halogenated 3-methyl-1-butene, ahalogenated 4-methyl-1-pentene, a halogenated 3-methyl-1-pentene, ahalogenated 3-ethyl-1-pentene, a halogenated 4,4-dimethyl-1-pentene, ahalogenated 4-methyl-1-hexene, a halogenated 4,4-dimethyl-1-hexene, ahalogenated 4-ethyl-1-hexene, and a halogenated 3-ethyl-1-hexene.

The above α-olefins may be used in a single kind, or may be combined intwo or more kinds.

In the present invention, particularly preferred are ethylene,propylene, 1-butene, 1-pentene, 1-hexene, 3-methyl-1-butene,3-methyl-1-pentene, 1-octene, 1-decene, 1-undecene, 1-dodecene,1-tetradecene, 1-hexadecene, 1-octadecene, 1-eicosene, norbornene,5-methyl-2-norbornene, tetracyclododecene, and hydroxylated-1-undecene.

In the present invention, a non-conjugated polyene may be combined asneeded.

The non-conjugated polyene has 5 to 20 carbon atoms, preferably 5 to 10carbon atoms; and examples thereof include 1,4-pentadiene,1,4-hexadiene, 1,5-hexadiene, 1,4-octadiene, 1,5-octadiene,1,6-octadiene, 1,7-octadiene, 2-methyl-1,5-hexadiene,6-methyl-1,5-heptadiene, 7-methyl-1,6-octadiene,4-ethylidene-8-methyl-1,7-nonadiene, 4,8-dimethyl-1,4,8-decatriene,dicyclopentadiene, cyclohexadiene, dicyclooctadiene, methylenenorbornene, 5-vinyl norbornene, 5-ethylidene-2-norbornene,5-methylene-2-norbornene, 5-vinylidene-2-norbornene,5-isopropylidene-2-norbornene,6-chloromethyl-5-isopropenyl-2-norbornene,2,3-diisopropylidene-5-norbornene,2-ethylidene-3-isopropylidene-5-norobornene, and2-propenyl-2,2-norbornadiene.

As the non-conjugated polyenes, preferred are 5-vinylidene-2-norborneneand 5-ethylidene-2-norbornene.

Other copolymerization components may be contained therein to the degreenot adversely affecting the object of the present invention; and theembodiments thereof are within a scope of the present invention.

In the present invention, in terms of flexibility, stress absorption,stress relaxation and the like, the linear α-olefins having 2 to 10carbon atoms are preferable; and ethylene, propylene, 1-butene,1-pentene, 1-hexene, and 1-octene are more preferable. In terms ofproviding high stress absorption and polyolefin modification property,ethylene and propylene are still more preferable; and propylene isparticularly preferable.

4-Methyl-1-pentene Copolymer (AA)

(a-1): A 4-methyl-1-pentene copolymer (AA) according to the presentinvention comprises:

5 to 95 wt % of a structural unit (i) derived from 4-methyl-1-pentene,and

5 to 95 wt % of a structural unit (ii) derived from at least one kind ofα-olefin selected from α-olefins having 2 to 20 carbon atoms excluding4-methyl-1-pentene, provided that the total of the structural units (i)and (ii) is 100 wt %.

(b-1) and (c-1): The copolymer (AA) comprises:

the structural unit (i) preferably in an amount of 10 to 90 wt %, morepreferably 18 to 90 wt %, still more preferably 25 to 90 wt %, mostpreferably 30 to 85 wt %, particularly preferably 40 to 85 wt %, and

the structural unit (ii) preferably in an amount of 10 to 90 wt %, morepreferably 10 to 82 wt %, still more preferably 10 to 75 wt %, mostpreferably 15 to 70 wt %, particularly preferably 15 to 60 wt %,provided that the total of the structural units (i) and (ii) is 100 wt%.

The copolymer (AA) may comprise other copolymerization components to thedegree not adversely affecting the object of the present invention; andthe embodiments thereof are within a scope of the present invention.

(a-2): The copolymer (AA) has an intrinsic viscosity [η], as measured in135° C. decalin, of 0.01 to 5.0 (dL/g), preferably 0.05 to 4.0 (dL/g),more preferably 0.1 to 3.0 (dL/g), still more preferably 0.5 to 2.5(dL/g). The use of a catalyst described later can provide the polymerwithout impairing the molecular weight distribution. The combined use ofhydrogen during polymerization, as described later, can control amolecular weight of the polymer and provide polymers having molecularweights ranging from low to high without limitation.

(a-3) The copolymer (AA) has a ratio (Mw/Mn) of a weight-averagemolecular weight (Mw) to a number-average molecular weight (Mn), asmeasured by gel permeation chromatography (GPC), in the range of 1.0 to3.5, preferably 1.5 to 3.0, more preferably 1.5 to 2.5. A large Mw/Mn,raising a concern in terms of the influence of a compositiondistribution and a low-molecular weight polymer, may not allow thepolymer to exhibit mechanical properties, moldability, and abrasionresistance, and may cause the polymer to have stickiness during moldingoperation. The Mw/Mn in the range of 1.5 to 2.5 is advantageous inexhibiting the above characteristics and thus is of a high industrialvalue. The use of a catalyst described later can provide the polymerhaving a Mw/Mn within the above range without impairing the molecularweight. If an application requires the 4-methyl-1-pentene copolymer (AA)to have a wide molecular weight distribution, this need can be satisfiedby blending polymers differing in molecular weight, or by employing amultistep polymerization method, or the like.

The copolymer (AA) has a weight-average molecular weight (Mw) in termsof polystyrene, as measured by gel permeation chromatography (GPC),preferably in the range of 500 to 10,000, 000, more preferably 1,000 to5,000,000, still more preferably 1,000 to 2,500,000.

(b-2): The copolymer (AA) has a difference (change) ΔHS in Shore Ahardness between immediately after the measurement and 15 seconds afterthe measurement being the range of 10 to 50, preferably 15 to 50, morepreferably 20 to 50, Shore A hardness being measured using a press sheetthereof having a thickness of 3 mm in accordance with JIS K6253. Theseranges are preferable in terms of stress absorption and stressrelaxation.

(b-3): The copolymer (AA) preferably has a melting point (Tm), asmeasured by DSC, of lower than 110° C. or not observed, more preferablylower than 100° C. or not observed, still more preferably lower than 85°C. or not observed. The melting point can be varied arbitrarily by typesand compositions of the comonomers. When the melting point is within theabove range, flexibility and toughness are excellent.

The copolymer (AA) has a maximum value of loss tangent tan δ, asobtained by measuring a dynamic viscoelasticity thereof within atemperature range of −70 and 180° C. at a frequency of 10 rad/s, beingwithin a temperature range of 0 to 40° C., the maximum value of tan δbeing 0.5 or more, preferably 1.0 or more, more preferably 1.5 or more.The copolymer having the above ranges is preferable because of havingexcellent stress absorption.

Examples of the α-olefin having 2 to 20 carbon atoms used in thecopolymer (AA), which examples exclude 4-methyl-1-pentene, includelinear or branched α-olefins, cyclic olefins, aromatic vinyl compounds,conjugated dienes, non-conjugated polyenes, and functionalized vinylcompounds.

The linear α-olefins are those having 2 to 20 carbon atoms, preferably 2to 15 carbon atoms, more preferably 2 to 10 carbon atoms, with examplesthereof including ethylene, propylene, 1-butene, 1-pentene, 1-hexene,1-octene, 1-decene, 1-undecene, 1-dodecene, 1-tetradecene, 1-hexadecene,1-octadecene and 1-eicosene; and ethylene, propylene, 1-butene,1-pentene, 1-hexene, and 1-octene are more preferable.

The branched α-olefins are those having 5 to 20 carbon atoms, preferably5 to 15 carbon atoms, with examples thereof including 3-methyl-1-butene,3-methyl-1-pentene, 3-ethyl-1-pentene, 4,4-dimethyl-1-pentene,4-methyl-1-hexene, 4,4-dimethyl-1-hexene, 4-ethyl-1-hexene, and3-ethyl-1-hexene.

The cyclic olefins are those having 3 to 20 carbon atoms, preferably 5to 15 carbon atoms, with examples thereof including cyclopentene,cyclohexene, cycloheptene, norbornene, 5-methyl-2-norbornene,tetracyclododecene, and vinylcyclohexane. With regard to the aromaticvinyl compounds, the conjugated dienes, the non-conjugated polyenes, thefunctionalized vinyl compounds and the like, the foregoing descriptionscan be referred to.

The above α-olefins may be used in a single kind, or may be combined intwo or more kinds.

In the present invention, particularly preferred are ethylene,propylene, 1-butene, 1-hexene, 3-methyl-1-butene, 3-methyl-1-pentene,1-octene, 1-decene, 1-undecene, 1-dodecene, 1-tetradecene, 1-hexadecene,1-octadecene, 1-eicosene, norbornene, 5-methyl-2-norbornene,tetracyclododecene, 5-vinylidene-2-norbornene, and5-ethylidene-2-norbornene.

Other copolymerization components may be contained therein to the degreenot adversely affecting the object of the present invention; and theembodiments thereof are within a scope of the present invention.

<Production Method>

Next, production methods of the 4-methyl-1-pentene/α-olefin copolymerand the 4-methyl-1-pentene copolymer, according to the presentinvention, are described.

To produce the copolymer according to the present invention, hithertoknown catalysts are favorably used, such as magnesium-supported titaniumcatalysts, and metallocene catalysts as described in WO-A-01/53369,WO-A-01/027124, JP-A-3-193796, and JP-A-02-41303. More preferably, anolefin polymerization catalyst containing a metallocene catalystrepresented by the following general formula (1) or (2) is favorablyused.

(In the formulae, R¹, R², R³, R⁴, R⁵, R⁶, R⁷, R⁸, R⁹, R¹⁰, R¹¹, R¹²,R¹³, and R¹⁴ are selected from hydrogen, hydrocarbon groups, andhydrocarbon groups containing silicon, and may be the same as ordifferent from each other; In R¹ to R⁴, adjacent substituents may bebonded to each other to form a ring; In R⁵ to R¹², adjacent substituentsmay be bonded to each other to form a ring;

A denotes a bivalent hydrocarbon group having 2 to 20 carbon atoms thatmay partially contain an unsaturated bond and/or an aromatic ring. A maycontain two or more ring structures which include a ring formed by A andY;

M denotes a metal selected from the Group 4 of the periodic table;

Y denotes carbon or silicon;

Q denotes a halogen, a hydrocarbon group, an anion ligand, or a neutralligand to which lone-pair electrons can coordinate; and Qs may be thesame as or different from each other; and

j denotes an integer of from 1 to 4.)

R¹, R², R³, R⁴, R⁵, R⁶, R⁷, R⁸, R⁹, R¹⁰, R¹¹, R¹², R¹³, and R¹⁴ in thegeneral formula (1) or (2) are selected from hydrogen, hydrocarbongroups, and hydrocarbon groups containing silicon, and may be the sameas or different from each other.

The hydrocarbon groups are preferably alkyl groups having 1 to 20 carbonatoms, arylalkyl groups having 7 to 20 carbon atoms, aryl groups having6 to 20 carbon atoms, or alkylaryl groups having 7 to 20 carbon atoms.The hydrocarbon group may have one or more ring structures. A part of oran entirety of the hydrocarbon group may be substituted with afunctional group such as a hydroxyl group, an amino group, a halogengroup and a fluorine-containing hydrocarbon group. Specific examplesinclude methyl, ethyl, n-propyl, isopropyl, 2-methylpropyl,1,1-dimethylpropyl, 2,2-dimethylpropyl, 1,1-diethylpropyl,1-ethyl-1-methylpropyl, 1,1,2,2-tetramethylpropyl, sec-butyl,tert-butyl, 1,1-dimethylbutyl, 1,1,3-trimethylbutyl, neopentyl,cyclohexylmethyl, cyclohexyl, 1-methyl-1-cyclohexyl, 1-adamantyl,2-adamantyl, 2-methyl-2-adamantyl, menthyl, norbornyl, benzyl,2-phenylethyl, 1-tetrahydronaphthyl, 1-methyl-1-tetrahydronaphthyl,phenyl, biphenyl, naphthyl, tolyl, chlorophenyl, chlorobiphenyl, andchloronaphthyl.

The hydrocarbon groups containing silicon are preferably alkylsilyl orarylsilyl groups each having 1 to 4 silicon atoms and 3 to 20 carbonatoms and specifically include trimethylsilyl, tert-butyldimethylsilyl,and triphenylsilyl.

The adjacent substituents in R⁵ to R¹² on the fluorene ring may bebonded to each other to form a ring. Examples of such a substitutedfluorenyl group include benzofluorenyl, dibenzofluorenyl,octahydrodibenzofluorenyl, and octamethyloctahydrodibenzofluorenyl.

The substituents in R⁵ to R¹² on the fluorene ring preferably displaybilateral symmetry, that is, R⁵=R¹², R⁶=R¹¹, R7=R¹⁰, and R⁸=R⁹ in termsof the easiness of synthesis. The fluorene ring is more preferablyunsubstituted fluorene, 3,6-disubstituted fluorene, 2,7-disubstitutedfluorene, or 2,3,6,7-tetrasubstituted fluorene. The positions 3, 6, 2,and 7 on the fluorene ring correspond to R⁷, R¹⁰, R⁶, and R¹¹,respectively.

R¹³ and R¹⁴ in the general formula (1) are selected from hydrogen andhydrocarbon groups and may be the same as or different from each other.As preferred specific examples of the hydrocarbon groups, thosedescribed above can be mentioned.

Y denotes carbon or silicon. In the general formula (1), R¹³ and R¹⁴ arebonded to Y to form a substituted methylene group or a substitutedsilylene group as a crosslinking portion. Preferred specific examplesinclude methylene, dimethyl methylene, diisopropyl methylene,methyl-tert-butyl methylene, dicyclohexyl methylene, methylcyclohexylmethylene, methylphenyl methylene, fluoromethylphenyl methylene,chloromethylphenyl methylene, diphenyl methylene, dichlorophenylmethylene, difluorophenyl methylene, methylnaphthyl methylene,dibiphenyl methylene, di-p-methylphenyl methylene, methyl-p-methylphenylmethylene, ethyl-p-methylphenyl methylene, dinaphthyl methylene ordimethyl silylene, diisopropyl silylene, methyl-tert-butyl silylene,dicyclohexyl silylene, methylcyclohexyl silylene, methylphenyl silylene,fluoromethylphenyl silylene, chloromethylphenyl silylene, diphenylsilylene, di-p-methylphenyl silylene, methyl-p-methylphenyl silylene,ethyl-p-methylphenyl silylene, methylnaphthyl silylene, and dinaphthylsilylene.

In the general formula (2), Y is bonded to A to form a cycloalkylidenegroup or a cyclomethylenesilylene group. A is a bivalent hydrocarbongroup having 2 to 20 carbon atoms that may partially contain anunsaturated bond and/or an aromatic ring. Preferred specific examplesinclude cyclopropylidene, cyclobutylidene, cyclopentylidene,cyclohexylidene, cycloheptylidene, bicyclo[3.3.1]nonylidene,norbornylidene, adamantylidene, tetrahydronaphthylidene,dihydroindanylidene, cyclodimethylenesilylene,cyclotrimethylenesilylene, cyclotetramethylenesilylene,cyclopentamethylenesilylene, cyclohexamethylenesilylene, andcycloheptamethylenesilylene.

M in the general formulae (1) and (2) denotes a metal selected from theGroup 4 of the periodic table. Examples of M include titanium,zirconium, and hafnium.

Q denotes a halogen, a hydrocarbon group having 1 to 20 carbon atoms, ananion ligand, or a neutral ligand to which lone-pair electrons cancoordinate. Qs may be the same as or different from each other. Specificexamples of the halogen include fluorine, chlorine, bromine, andiodine.Specific examples of the hydrocarbon group include those describedabove. Specific examples of the anion ligand include alkoxy groups, suchas methoxy, tert-butoxy, and phenoxy, carboxylate groups, such asacetates and benzoates, and sulfonate groups, such as mesylates andtosylates. Specific examples of the neutral ligand to which lone-pairelectrons can coordinate include organophosphorus compounds, such astrimethylphosphine, triethylphosphine, triphenylphosphine, anddiphenylmethylphosphine, and ethers, such as tetrahydrofuran, diethylether, dioxane, and 1,2-dimethoxyethane. Qs may be the same as ordifferent from each other. Preferably, at least one of Qs is a halogenor an alkyl group.

As specific examples of the metallocene compound in the presentinvention, preferred examples include compounds exemplified inWO-A-01/027124, WO-A-2006/025540, or WO-A-2007/308607. However, thesecompounds do not limit the scope of the present invention.

When using the metallocene catalyst for the production of the copolymeraccording to the present invention, the catalyst component comprises:

a metallocene compound (A) (for example, the metallocene compoundrepresented by the general formula (1) or (2));

at least one compound (B) selected from:

an organoaluminum compound (B-1),

an organoaluminum oxy-compound (B-2), and

a compound (B-3) that reacts with the metallocene compound (A) to forman ion pair;

and, if necessary,

a fine particulate carrier (C).

As a production method, for example, a method described inWO-A-01/027124 is adoptable.

As specific examples of at least one compound (B) selected from theorganoaluminum compound (B-1), the organoaluminum oxy-compound (B-2) andthe compound (B-3) that reacts with the metallocene compound (A) to forman ion pair, and the fine particulate carrier (C), there can bementioned compounds and carriers hitherto known as these components inthe field of olefin polymerization, such as specific examples describedin WO-A-01/027124.

In the present invention, polymerization can be performed byliquid-phase polymerization method, such as solution polymerization andsuspension polymerization, or by gas-phase polymerization method.

In the liquid-phase polymerization method, an inert hydrocarbon solventmay be used, with specific examples including aliphatic hydrocarbons,such as propane, butane, pentane, hexane, heptane, octane, decane,dodecane, and kerosene; alicyclic hydrocarbons, such as cyclopentane,cyclohexane, and methylcyclopentane; aromatic hydrocarbons, such asbenzene, toluene, and xylene; halogenated hydrocarbons, such as ethylenechloride, chlorobenzene, dichloromethane, trichloromethane andtetrachloromethane; and mixtures thereof.

Furthermore, bulk polymerization using 4-methyl-1-pentene and anα-olefin as a solvent can be performed.

Moreover, in the present invention, multistep polymerization in whichpolymerization conditions are varied between steps to obtain a copolymerwith controlled composition distribution can be performed.

In polymerization, the amount of the component (A) usually ranges from10⁻⁸ to 10⁻² mol, preferably 10⁻⁷ to 10⁻³ mol, in terms of a metal atomof the Group 4 of the periodic table, per 1 L of reaction volume. Theamount of the component (B-1) is such that the molar ratio [(B-1)/M] ofthe component (B-1) to a transition metal atom (M) in the component (A)usually ranges from 0.01 to 5000, preferably 0.05 to 2000. The amount ofthe component (B-2) is such that the molar ratio [(B-2)/M] of thecomponent (B-2) to a transition metal atom (M) in the component (A)usually ranges from 10 to 5000, preferably 20 to 2000. The amount of thecomponent (B-3) is such that the molar ratio [(B-3)/M] of the component(B-3) to a transition metal atom (M) in the component (A) usually rangesfrom 1 to 10, preferably 1 to 5.

The polymerization temperature usually ranges from −50 to 200° C.,preferably 0 to 150° C., more preferably 20 to 100° C.

The polymerization pressure usually ranges from ordinary pressure to agauge pressure of 10 MPa, preferably from ordinary pressure to a gaugepressure of 5 MPa. The polymerization reaction can be performed by anyprocess of batch, semicontinuous and continuous processes. Thepolymerization can be performed also in two or more steps differing inreaction conditions.

In polymerization, hydrogen may be added to control the molecular weightof a polymer to be generated, or polymerization activity. The amount ofhydrogen ranges from about 0.001 to 100 NL per 1 kg of the copolymer.

In the copolymer according to the present invention, part of thecopolymer may be graft modified with a polar monomer. Examples of thepolar monomer include ethylenic unsaturated compounds containing ahydroxyl group, ethylenic unsaturated compounds containing an aminogroup, ethylenic unsaturated compounds containing an epoxy group,aromatic vinyl compounds, unsaturated carboxylic acids or derivativesthereof, vinyl ester compounds, vinyl chloride, organosilicon compoundscontaining a vinyl group, and carbodiimide compounds.

As the polar monomer, particularly preferred are unsaturated carboxylicacids or derivatives thereof, and organosilicon compounds containing avinyl group.

Examples of the unsaturated carboxylic acids or derivatives thereofinclude unsaturated compounds having at least one carboxylic acid group,esters of the compounds having a carboxylic acid group and alkylalcohols, and unsaturated compounds having at least one carboxylic acidanhydride group. Examples of the unsaturated group include a vinylgroup, a vinylene group, and an unsaturated cyclic hydrocarbon group. Asthese compounds, those hitherto known can be used without particularlimitation. Specific examples thereof include unsaturated carboxylicacids such as (meth)acrylic acid, maleic acid, fumaric acid,tetrahydrophthalic acid, itaconic acid, citraconic acid, crotonic acid,isocrotonic acid, and nadic acid [trademark](endocis-bicyclo[2.2.1]hepto-5-en-2,3-dicarboxylic acid); or derivativesthereof such as acid halides, amides, imides, anhydrides and esters.Specific examples of the derivatives include methyl acrylate, methylmethacrylate, dimethyl maleate, monomethyl maleate, dimethyl fumarate,dimethyl itaconate, diethyl citraconate, dimethyl tetrahydrophthalate,dimethyl nadicate (dimethylendocis-bicyclo[2,2,1]hepto-5-en-2,3-dicarboxylate), malenyl chloride,maleimide, maleic anhydride, citraconic anhydride, monomethyl maleate,dimethyl maleate, and glycidyl maleate. These unsaturated carboxylicacids and derivatives thereof may be used in a single kind, or may becombined in two or more kinds. Of these, unsaturated dicarboxylic acidsor acid anhydrides thereof are preferred. In particular, maleic acid,nadic acid [trademark], or acid anhydrides thereof are preferably used.

As the organosilicon compounds containing a vinyl group, hitherto knowncompounds are employable without particular limitation. Specificemployable examples include vinyltriethoxysilane, vinyltrimethoxysilane,vinyltris(β-methoxy-ethoxysilane), γ-glycidoxypropyl trimethoxysilane,γ-aminopropyltriethoxysilane, γ-methacryloxypropyltrimethoxysilane,2-(3,4-epoxycyclohexyl)ethyltrimethoxysilane,3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethylethoxysilane,p-styryltrimethoxysilane, 3-methacryloxypropylmethyldimethoxysilane,3-methacryloxypropylmethyldiethoxysilane,3-methacryloxypropyltriethoxysilane, 3-acryloxypropyltrimethoxysilane,N-2-(aminoethyl)-3-aminopropylmethyldimethoxysilane,N-2-(aminoethyl)-3-aminopropyltrimethoxysilane,N-2-(aminoethyl)-3-aminopropyltriethoxysilane,3-aminopropyltrimethoxysilane,3-triethoxysilyl-N-(1,3-dimethyl-butylidene)propylamine,N-phenyl-3-aminopropyltrimethoxysilane, 3-ureidopropyltriethoxysilane,and 3-isocyanatepropyltriethoxysilane. Preferred examples includeγ-glycidoxypropyl trimethoxysilane, γ-aminopropyltriethoxysilane,γ-methacryloxypropyltrimethoxysilane, vinyltriethoxysilane,vinyltrimethoxysilane, and 3-acryloxypropyltrimethoxysilane. Morepreferred examples include vinyltriethoxysilane, vinyltrimethoxysilane,and 3-acryloxypropyltrimethoxysilane, which have small steric hindranceand high graft modification efficiency.

The polar monomer is used usually in an amount of 1 to 100 parts byweight, preferably 5 to 80 parts by weight based on 100 parts by weightof the copolymer according to the present invention.

The polar monomer may be used in a single kind, or may be combined intwo or more kinds.

This graft polymerization is carried out usually in the presence of aradical initiator.

As the radical initiator, organic peroxides, azo compounds, or the likeare employable.

Specific examples thereof include:

dialkyl peroxides such as dicumyl peroxide, di-t-butyl peroxide,di-t-butylperoxy-3,3,5-trimethylcyclohexane, t-butylcumyl peroxide,di-t-amyl peroxide, t-butylhydroperoxide,2,5-dimethyl-2,5-di(t-butylperoxy)hexyne-3,2,5-dimethyl-2,5-di(benzoylperoxy) hexane, 2,5-dimethyl-2,5-di(t-butylperoxy) hexane, andα,α′-bis(t-butylperoxy-m-isopropyl)benzene;

peroxyesters such as t-butylperoxyacetate, t-butylperoxyisobutylate,t-butylperoxypivalate, t-butylperoxymaleic acid,t-butylperoxyneodecanoate, t-butylperoxybenzoate, anddi-t-butylperoxyphthalate;

ketone peroxides such as dicyclohexanone peroxide; and mixtures thereof.

The radical initiator may be directly mixed with the copolymer and thepolar monomer and then used, but may be dissolved in a slight amount ofan organic solvent and then used. This organic solvent is notparticularly limited as long as being an organic solvent capable ofdissolving the radical initiator.

In the graft polymerization with the polar monomer, a reductivesubstance may be used. The use of the reductive substance can improvethe graft amount of the polar monomer.

The graft polymerization can be performed by hitherto known methods, forexample in such a manner that the copolymer is dissolved in an organicsolvent, and into the solution, the polar monomer, the radical initiatorand the like are added; and then the resultant solution is reacted at atemperature of 60 to 200° C., preferably 80 to 260° C., for 0.5 to 15hours, preferably 1 to 10 hours.

Alternatively, the copolymer can be reacted with the polar monomer withno solvent using an extruder or the like. This reaction is desirablyperformed usually for 0.5 to 10 minutes, usually at a temperature whichis a melting point or higher of the ethylene polymer, specifically at atemperature of 120 to 250° C.

The modification amount of the copolymer thus obtained (the graft amountof the polar monomer) is usually 0.1 to 50 wt %, preferably 0.2 to 30 wt%, more preferably 0.2 to 10 wt %.

In the present invention, when the copolymer comprises the graftmodified copolymer, the copolymer has excellent adhesion andcompatibility with other resins, and can provide surfaces of articleswith improved wetting property.

The graft modified copolymer, through being crosslinked, can be usedfavorably for crosslinked wires and crosslinked pipes.

In crosslinking at least a part of or an entirety of the copolymer usinga crosslinking agent, the crosslinking agent is not particularlylimited, and examples thereof include sulfur, organic peroxides, and SiHgroup-containing compounds.

Examples of the crosslinking agent include organic peroxides such asdicumyl peroxide, 2,5-dimethyl-2,5-tert-butylperoxyhexyne, sulfur, andmorpholine disulfide. These may be used together with crosslinkingassistants such as stearic acid and zinc oxide.

If sulfur is used, sulfur is used preferably in an amount of 0.1 to 10parts by weight based on 100 parts by weight of the copolymer. If theorganic peroxide is used, the organic peroxide is used preferably in anamount of 0.05 to 15 parts by weight based on 100 parts by weight of thecopolymer. If the SiH group-containing compound is used, the SiHgroup-containing compound is used in an amount of 0.2 to 20 parts byweight, preferably in an amount of 0.5 to 10 parts by weight, mostpreferably in an amount of 0.5 to 5 parts by weight based on 100 partsby weight of the copolymer. The use of the SiH group-containing compoundmay be the addition of a catalyst, and as an optional component, asilane coupling agent and/or a reaction inhibitor.

In the present invention, the copolymer may have a nucleating agentblended therein, in order to further improve its moldability, i.e., inorder to raise the crystallization temperature and increase thecrystallization rate. Examples of the nucleating agent includedibenzylidene sorbitol-based nucleating agents, phosphate-basednucleating agents, rosin-based nucleating agents, benzoic acid metalsalt-based nucleating agents, fluorinated polyethylene,2,2-methylenebis(4,6-di-t-butylphenyl)sodium phosphate, pimelic acid anda salt thereof, and 2,6-naphthalene acid dicarboxylic aciddicyclohexylamide. The blending amount is not particularly limited, butis preferably 0.1 to 1 part by weight based on 100 parts by weight ofthe copolymer. The nucleating agent can be arbitrarily added duringpolymerization, after polymerization, or in mold processing.

The copolymer according to the present invention may have additivesblended therein, such as weathering stabilizers, heat stabilizers,anti-static agents, anti-slip agents, anti-blocking agents, blowingagents, crystallization assistants, anti-fogging agents, (transparent)nucleating agents, lubricants, pigments, dyes, plasticizers, anti-agingagents, hydrochloric acid absorbents, antioxidants, releasing agents,impact modifiers, anti-UV agents (ultraviolet absorbents), fillers,crosslinking agents, co-crosslinking agents, crosslinking assistants,adhesives, softeners, flame retardants, and processing assistants,according to necessity, to the degree not adversely affecting theproperties of the modified product.

Specific examples of the additives include 2,6-di-t-butyl-p-cresol,tetrakis[methylene-3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate]methane,4,4′-butylidenebis(6-t-butyl-m-cresol), tocophenols, ascorbic acid,dilauryl thiodipropionate, phosphoric acid based stabilizers, fatty acidmonoglyceride, N,N-[bis-2-hydroxyethyl]alkylamines,2-(2′-hydroxy-3′,5′-di-t-butylphenyl)-5-chlorobenzotriazole, calciumstearate, magnesium oxide, magnesium hydroxide, alumina, aluminumhydroxide, silica, clay, gypsum, glass fibers, titania, calciumcarbonate, and carbon black.

As the softeners, softeners hitherto known are employable, with examplesincluding:

Petroleum-based substances, such as process oil, lubricating oil,paraffins, liquid paraffin, polyethylene wax, polypropylene wax,petroleum asphalt and vaseline;

coal tars, such as coal tar and coal tar pitch;

fatty oils, such as castor oil, linseed oil, rapeseed oil, soybean oiland coconut oil;

waxes, such as tall oil, beeswax, carnauba wax and lanolin; fatty acids,such as ricinolic acid, palmitic acid, stearic acid, 12-stearatehydroxide, montanic acid, oleic acid, and erucic acid, or metal saltsthereof;

synthetic polymer materials, such as petroleum resins, coumarone-indeneresins and atactic polypropylene;

ester-based plasticizers, such as dioctyl phthalate, dioctyladipate anddioctylsebacate;

others, such as microcrystalline wax, liquid polybutadiene, modifiedproducts or hydrogenated products thereof; and liquid thiokol.

4-Methyl-1-pentene/α-olefin copolymer compositions (X), (X11), (X12),(X21), and (X22)

A 4-methyl-1-pentene/α-olefin copolymer composition (X) according to thepresent invention comprises: 5 to 95 parts by weight, preferably 10 to90 parts by weight, more preferably 20 to 80 parts by weight of the4-methyl-1-pentene/α-olefin copolymer (A), and 95 to 5 parts by weight,preferably 90 to 10 parts by weight, more preferably 80 to 20 parts byweight of a thermoplastic resin (B) described later, provided that thetotal of (A) and (B) is 100 parts by weight.

The composition comprising the copolymer and the resin within the aboveranges is excellent in moldability, flexibility, vibration dampingproperties, stress absorption, scratch resistance, abrasion resistance,mechanical properties, and toughness.

A 4-methyl-1-pentene/α-olefin copolymer composition (X11) or (X12)comprises:

a 4-methyl-1-pentene/α-olefin copolymer satisfying at least therequirements (a) to (d) and comprising 10 to 32 mol %, preferably 15 to32 mol % of the structural unit (i), 68 to 90 mol %, preferably 68 to 85mol % of the structural unit (ii), and 0 to 10 mol % of the structuralunit (iii), provided that the total of the structural units (i), (ii),and (iii) is 100 mol %, and a thermoplastic resin (B), in theabove-described ranges.

In terms of flexibility and mechanical properties, it is preferable thatthe copolymer composition (X11) comprises:

50 to 95 parts by weight, preferably 55 to 90 parts by weight, morepreferably 60 to 80 parts by weight of the copolymer (A), and

5 to 50 parts by weight, preferably 10 to 45 parts by weight, morepreferably 20 to 40 parts by weight of the thermoplastic resin (B)described later, provided that the total of (A) and (B) is 100 parts byweight.

In terms of providing excellent stress absorption, it is preferable thatthe copolymer composition (X11) satisfies the following requirement(j1).

(j1): The maximum value of loss tangent tan δ, as obtained by measuringa dynamic viscoelasticity thereof within a temperature range of −70 to180° C. at a frequency of 10 rad/s, is within a temperature range of −70to 180° C., preferably −50 to 40° C., more preferably −20 to 40° C., andthe maximum value of tan δ is 0.4 or more, preferably 0.4 to 5.0, morepreferably 0.5 to 5.0, still more preferably 0.7 to 5.0.

In terms of providing flexibility and mechanical properties, it ispreferable that the copolymer composition (X11) satisfies the followingrequirement (e1).

(e1): The change ΔHS in Shore A hardness between immediately after themeasurement and 15 seconds after the measurement is 5 to 50, preferably8 to 50.

In terms of heat resistance and mechanical properties, it is preferablethat the copolymer composition (X12) comprises:

5 parts by weight to less than 49 parts by weight, preferably 5 parts byweight to less than 40 parts by weight, more preferably 10 parts byweight to less than 30 parts by weight of the copolymer, and

51 to 95 parts by weight, preferably 60 to 95 parts by weight, morepreferably 70 to 90 parts by weight of the thermoplastic resin (B)described later, provided that the total of the copolymer and thethermoplastic resin (B) is 100 parts by weight.

In addition, it is preferable that the composition (X12) satisfies thefollowing requirements.

(f): The softening temperature is in the range of 100 to 250° C.,preferably 105 to 250° C.

(g): The tensile modulus (YM) is 300 to 2000 MPa, preferably 400 to 2000MPa, more preferably 500 to 1800 MPa.

The composition having a softening temperature and a tensile modulusbeing within the above ranges is excellent in e.g., heat resistance,toughness and surface tension. The softening temperature can becontrolled by e.g., compositional ratio in each composition. Thecomposition having a softening temperature within the above range isexcellent in e.g., heat resistance, toughness and mechanical properties.

In terms of providing flexibility and mechanical properties, it is morepreferable that the copolymer composition (X11 or X12) further satisfiesthe following requirement (hl).

(h1): The melting point [Tm], as measured by differential scanningcalorimetry (DSC), is observed within a temperature range of 50 to 250°C., more preferably in the range of 70 to 250° C.

A 4-methyl-1-pentene/α-olefin copolymer composition (X21) or (X22)comprises:

a 4-methyl-1-pentene/α-olefin copolymer satisfying at least therequirements (a) to (d) and comprising 33 to 80 mol %, preferably 50 to75 mol % of the structural unit (i), 67 to 20 mol %, preferably 50 to 25mol % of the structural unit (ii), and 0 to 10 mol %, preferably 0 to 5mol % of the structural unit (iii), provided that the total of thestructural units (i), (ii), and (iii) is 100 mol %, and

a thermoplastic resin (B), in the above-described ranges.

In terms of heat resistance, stress relaxation, stress absorption, andmechanical properties, it is preferable that the copolymer composition(X21) comprises:

50 parts by weight to less than 95 parts by weight, preferably 55 to 90parts by weight, more preferably 60 to 80 parts by weight of thecopolymer, and

5 to 50 parts by weight, preferably 10 to 45 parts by weight, morepreferably 20 to 40 parts by weight of the thermoplastic resin (B)described later, provided that the total of the copolymer and thethermoplastic resin (B) is 100 parts by weight.

In terms of providing excellent stress relaxation, the copolymercomposition (X21) satisfies any one or more of Shore A hardness andShore D hardness in the flowing requirement (e2).

(e2): The difference ΔHS in Shore A hardness defined by the followingequation (measured using a press sheet thereof having a thickness of 3mm in accordance with JIS K6253) is 10 to 50, preferably 15 to 50, morepreferably 20 to 50; or

the difference ΔHS in Shore D hardness between immediately after thestarting of indenter contact and 15 seconds after the starting ofindenter contact is 5 to 50, preferably 8 to 50, more preferably 10 to50.

ΔHS=(Shore A or D hardness immediately after the starting of indentercontact−Shore A or D hardness 15 seconds after the starting of indentercontact).

In terms of flexibility and mechanical properties, it is preferable thatthe copolymer composition (X22) comprises:

5 to 49 parts by weight, preferably 5 to less than 40 parts by weight,more preferably 10 to less than 30 parts by weight of the copolymer (A),and

50 to 95 parts by weight, preferably 60 to 95 parts by weight, morepreferably 70 to 90 parts by weight of the thermoplastic resin (B)described later, provided that the total of (A) and (B) is 100 parts byweight.

<Thermoplastic Resin (B)>

The thermoplastic resin (B) used in the present invention is notparticularly limited as long as being different from the4-methyl-1-pentene/α-olefin copolymer according to the present inventionand the 4-methyl-1-pentene copolymer according to the present invention.Examples thereof include resins described below. In the presentinvention, the examples of the thermoplastic resin (B) includeelastomers and copolymer rubbers.

Thermoplastic polyolefin resins (excluding the polymers according to thepresent invention; and the same is applied hereinafter), such aslow-density polyethylene, medium-density polyethylene, high-densitypolyethylene, low-density polyethylene by high pressure process,isotactic polypropylene, syndiotactic polypropylene, poly(1-butene),poly(4-methyl-1-pentene), poly(3-methyl-1-butene), ethylene/α-olefincopolymers, propylene/α-olefin copolymers, 1-butene/α-olefin copolymers,cyclic olefin copolymers, and chlorinated polyolefins;

thermoplastic polyamide resins, such as aliphatic polyamides (nylon 6,nylon 11, nylon 12, nylon 66, nylon 610, and nylon 612);

thermoplastic polyester resins, such as polyethylene terephthalate,polybutylene terephthalate, and polyester elastomers;

thermoplastic vinyl aromatic resins, such as polystyrene, ABS resin, ASresin, styrene-based elastomers (styrene/butadiene/styrene blockpolymer, styrene/isoprene/styrene block polymer,styrene/isobutylene/styrene block polymer, and hydrogenated products ofthe above polymers);

thermoplastic polyurethanes; vinyl chloride resin; vinylidene chlorideresin; acryl resin; ethylene/vinyl acetate copolymer;ethylene/methacrylate (acrylate) copolymer; ionomers; ethylene/vinylalcohol copolymers; polyvinyl alcohols; fluorine-based resinpolycarbonates; polyacetals; polyphenylene oxide; polyphenylene sulfidepolyimides; polyarylates; polysulfones; polyether sulfones; rosin-basedresins; terpene-based resins; and petroleum resins, and

copolymer rubbers, such as ethylene/α-olefin/diene copolymers,propylene/α-olefin/diene copolymers, 1-butene/α-olefin/diene copolymers,polybutadiene rubber, polyisoprene rubber, neoprene rubber, nitrilerubber, butyl rubber, polyisobutylene rubber, natural rubbers, andsilicone rubber.

Examples of the polypropylene include an isotactic polypropylene and asyndiotactic polypropylene. The isotactic polypropylene may be ahomopolypropylene, a random copolymer of propylene with an α-olefinhaving 2 to 20 carbon atoms (excluding propylene), or a propylene blockcopolymer.

The poly(4-methyl-1-pentene) herein is different from theabove-described copolymer, and examples thereof include a4-methyl-1-pentene homopolymer, and a4-methyl-1-pentene/α-olefin randomcopolymer containing 4-methyl-1-pentene in an amount of 80 to 99.9 wt %,preferably 90 to 99.9 wt % and an α-olefin having 2 to 20, preferably 6to 20 carbon atoms, in an amount of 0.1 to 20 wt %, preferably 0.1 to 10wt %. In the case of the 4-methyl-1-pentene/α-olefin random copolymer,examples of the α-olefin to be copolymerized with 4-methyl-1-penteneinclude an α-olefin having 2 to 20, preferably 6 to 20 carbon atoms,such as ethylene, propylene, 1-butene, 1-hexene, 1-octene, 1-decene,1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene, and 1-eicosene.These may be used in a single kind or in a combination of two or morekinds. The poly(4-methyl-1-pentene) desirably has a melt flow rate (MFR;ASTM D1238, 260° C., 5.0 kg load) of 0.1 to 200 g/10 minutes, preferably1 to 150 g/10 minutes. The poly(4-methyl-1-pentene) may be acommercially available product, with examples thereof including TPX(trade name, manufactured by Mitsui Chemicals, Inc.) Products ofpoly(4-methyl-1-pentene) available from other manufacturers can besuitably used as long as satisfying the above requirement.

Examples of the polyethylene employable include those produced by ahitherto known technique, such as low-density polyethylene,medium-density polyethylene, high-density polyethylene, and low-densitypolyethylene by high pressure process.

The polybutene is a 1-butene homopolymer, or a copolymer of 1-butene andan olefin excluding 1-butene. Examples of the olefin are those describedabove, and these olefins are used in a single kind, or are combined intwo or more kinds. Examples of the copolymer include 1-butene/ethylenerandom copolymer, 1-butene/propylene random copolymer,1-butene/methylpentene copolymer, 1-butene/methylbutene copolymer, and1-butene/propylene/ethylene copolymer. In these copolymers, in terms ofheat resistance, the content of 1-butene is preferably 50 mol % or more,more preferably 70 mol % or more, most preferably 85 mol % or more.

Examples of the rosin-based resin include natural rosins, polymerizedrosins, rosins modified with maleic acid, fumaric acid, (meth)acrylicacid or the like, and rosin derivatives. Examples of the rosinderivatives include esterified compounds of the natural rosins, thepolymerized rosins or the modified rosins; phenol-modified compounds ofthese rosins; esterified compounds thereof; and hydrogenated products ofthese rosins.

Examples of the terpene-based resins include resins composed of, e.g.,α-pinene, β-pinene, limonene, dipentene, terpene phenol, terpenealcohols and terpene aldehyde; aromatic-modified terpene-based resinsobtained by polymerizing α-pinene, β-pinene, limonene, dipentene or thelike, with an aromatic monomer such as styrene; and hydrogenatedproducts of these resins.

Examples of the petroleum resins include aliphatic petroleum resinsobtained using a C5 fraction of a tar naphtha as a main raw material,aromatic petroleum resins obtained using a C9 fraction of a tar naphthaas a main raw material, and copolymerized petroleum resins thereof:i.e., C5 petroleum resins (resins obtained by polymerizing the C5fraction of a naphtha crack oil), C9 petroleum resins (resins obtainedby polymerizing the C9 fraction of a naphtha crack oil), and C5-C9copolymerized petroleum resins (resins obtained by copolymerizing the C5fraction and the C9 fraction of a naphtha crack oil). Further examplesinclude coumarone/indene resins containing e.g., styrenes, indenes,coumarone, and dicyclopentadiene, as a tar naphtha fraction; alkylphenol resins represented by a condensation product between p-tert-butylphenol and acetylene; and xylene resins obtained by reacting o-xylene,p-xylene, or m-xylene with formalin.

It is preferable that one or more kinds of resins selected from thegroup consisting of the rosin-based resin, the terpene-based resin andthe petroleum resin are hydrogenated derivatives thereof, which haveexcellent weather resistance and discoloration resistance. The-abovedescribed resin has a softening temperature, as measured by aring-and-ball method, preferably in the range of 40 to 180° C. The-abovedescribed resin has a number-average molecular weight (Mn), as measuredby GPC, preferably in the range of about 100 to 10,000. One or morekinds of resins selected from the group consisting of the rosin-basedresin, the terpene-based resin, and the petroleum resin may becommercially available products.

Further, these resins may be commercially available products.

Among these thermoplastic resins (B), preferable resins are low-densitypolyethylene, medium-density polyethylene, high-density polyethylene,low-density polyethylene by high pressure process, isotacticpolypropylene, syndiotactic polypropylene, poly(1-butene),poly(4-methyl-1-pentene), poly(3-methyl-1-pentene), ethylene/α-olefincopolymers, propylene/α-olefin copolymers, 1-butene/α-olefin copolymers,styrene-based elastomers, vinyl acetate copolymer, ethylene/methacrylate(acrylate) copolymer, ionomers, fluorine-based resins, rosin-basedresins, terpene-based resins, and petroleum resins. In terms ofimprovement of heat resistance and low-temperature resistance, andflexibility, more preferred are polyethylene, isotactic polypropylene,syndiotactic polypropylene, poly(1-butene), poly(4-methyl-1-pentene),ethylene/α-olefin copolymers, propylene/α-olefin copolymers,1-butene/α-olefin copolymers, vinyl acetate copolymer, styrene-basedelastomers, rosin-based resins, terpene-based resins, and petroleumresins.

In the copolymer composition of the present invention, thesethermoplastic resins can be used in a single kind, or may be combined intwo or more kinds.

In the present invention, as the thermoplastic resin (B), it ispreferable to use a crystalline olefin resin (B1) in terms of heatresistance and moldability. In the present invention, “a crystallineolefin resin” means a resin having a melting point as measured by DSC of70° C. or higher.

The density of the resin (B1), although not particularly limited, ispreferably 0.850 g/cm³ or higher, more preferably 0.855 g/cm³ or higher,still more preferably 0.870 to 0.980 g/cm³ (ASTM D1505).

The crystalline olefin resins (B1) are, among the above-describedthermoplastic resins (B), particularly those having a crystallinity; andexamples thereof include low-density polyethylene, medium-densitypolyethylene, high-density polyethylene, low-density polyethylene byhigh pressure process, isotactic polypropylene, syndiotacticpolypropylene, poly(1-butene), poly(4-methyl-1-pentene),poly(3-methyl-1-pentene), ethylene/α-olefin copolymers,propylene/α-olefin copolymers, 1-butene/α-olefin copolymers, andstyrene-based elastomers; and preferable examples include polypropylene,poly(4-methyl-1-pentene), polyethylene, and polybutene.

<Graft Modification>

With regard to the 4-methyl-1-pentene/α-olefin copolymer compositions(X) to (X22) of the present invention, at least a part or an entiretythereof may be graft-modified with a polar monomer.

For example, a part or an entirety of the copolymer according to thepresent invention may be graft modified, apart or an entirety of theresin (B) according to the present invention may be graft modified, or apart or an entirety of each of the copolymer and the resin (B) accordingto the present invention may be graft modified.

With regard to the polar monomer to be used, the foregoing descriptionscan be referred to.

With regard to the polar monomer, an unsaturated carboxylic acid or aderivative thereof is preferable. With regard to the unsaturatedcarboxylic acid or the derivative thereof, the foregoing descriptionscan be referred to.

The polar monomer is used usually in an amount of 1 to 100 parts byweight, preferably 5 to 80 parts by weight, based on 100 parts by weightof a product to be modified. This graft polymerization is carried outusually in the presence of a radical initiator. With regard to theradical initiator, the foregoing descriptions can be referred to.

When the product to be modified is graft-polymerized with the polarmonomer, a reductive substance may be used. The use of the reductivesubstance can improve the graft amount of the polar monomer.

The graft polymerization can be performed by hitherto known methods, forexample in such a manner that the product to be modified is dissolved inan organic solvent, and into the solution, the polar monomer, theradical initiator and the like are added; and then the resultantsolution is reacted at a temperature of 40 to 250° C., preferably 60 to200° C., for 0.5 to 20 hours, preferably 1 to 15 hours.

The graft amount of the modified product thus obtained is usually 0.1 to50 wt %, preferably 0.2 to 30 wt %, more preferably 0.2 to 20 wt %,based on 100 wt % of the modified product.

The graft-modified copolymer composition may have polymers other thanthe 4-methyl-1-pentene/α-olefin copolymer, the 4-methyl-1-pentenecopolymer, and the thermoplastic resin (B) of the present invention,blended therein, such as thermoplastic resins and elastomers, to thedegree not adversely affecting the properties of the modified product.They may be blended in a graft modification step or be mixed after themodification.

<Crosslinking>

At least a part or an entirety of the copolymer compositions (X) to(X22) of the present invention may be crosslinked with a crosslinkingagent. The crosslinking agent is not particularly limited, with examplesthereof including sulfur, organic peroxides, and SiH-containingcompounds. With regard to the crosslinking method and the crosslinkingagent, the foregoing descriptions can be referred to.

<Additives>

The copolymer composition according to the present invention may havevarious additives blended therein in molding operation, to the degreenot adversely affecting the object of the present invention. With regardto the additives, the foregoing descriptions can be referred to.

The copolymer composition according to the present invention may furthercomprise thermoplastic resins other than the 4-methyl-1-pentene/α-olefincopolymer, the 4-methyl-1-pentene copolymer and the thermoplastic resin(B) of the present invention, to the degree not adversely affecting theobject of present invention. With regard to the other thermoplasticresins, the same resin as the resin (B) can be used.

4-Methyl-1-pentene Copolymer Composition (Y)

A 4-methyl-1-pentene copolymer composition (Y) according to the presentinvention comprises:

50 to 98 parts by weight, preferably 50 to 96 parts by weight, morepreferably 50 to 90 parts by weight of the 4-methyl-1-pentene copolymer(AA),

1 to 49 parts by weight, preferably 2 to 48 parts by weight, morepreferably 5 to 45 parts by weight of a crystalline olefin resin (BB)(melting point of 100° C. or higher) other than the 4-methyl-1-pentenecopolymer (AA), and

1 to 49 parts by weight, preferably 2 to 48 parts by weight, morepreferably 5 to 45 parts by weight of an α-olefin copolymer (CC)(melting point of lower than 100° C.) other than the 4-methyl-1-pentenecopolymer (AA), provided that the total of (AA), (BB), and (CC) is 100parts by weight.

The copolymer composition with the components contained within the aboveranges is preferable, particularly because of having excellentmoldability, and further because of having excellent flexibility,vibration damping properties, stress absorption, scratch resistance,abrasion resistance, mechanical properties, and toughness.

In terms of flexibility and stress relaxation, it is preferable that thecopolymer composition (Y) has:

a difference ΔHS in Shore A hardness between immediately after thestarting of indenter contact and 15 seconds after the starting ofindenter contact being 10 to 50, more preferably 15 to 50, still morepreferably 20 to 50 (Shore A hardness is measured using a press sheetthereof having a thickness of 3 mm in accordance with JIS K6253); or

a difference ΔHS in Shore D hardness between immediately after thestarting of indenter contact and 15 seconds after the starting ofindenter contact being 5 to 50, more preferably 8 to 50, still morepreferably 10 to 50 (Shore D hardness is measured using a press sheetthereof having a thickness of 3 mm in accordance with JIS K6253).

It is preferable that the composition (Y) satisfies any one or more ofΔHS in Shore A hardness and ΔHS in Shore D hardness.

The copolymer composition (Y) preferably has a ball drop resilienceratio, as obtained by dropping a rigid ball of 16.310 g from a height of460 mm under a room temperature of 25° C. in accordance with JIS K6400,of 30% or less, more preferably 28% or less, still more preferably 25%or less.

The ball drop resilience ratio can be controlled by comonomercompositional ratio in the copolymer (AA), mixing ratio in the copolymercomposition (Y), and the like. For example, when the content of4-methyl-1-pentene in the copolymer (AA) is 85 wt % or less, vibrationdamping properties and stress relaxation are excellent.

The copolymer composition (Y) has a peak value of loss tangent (tan δ)due to a glass transition temperature, as obtained by measuringtemperature dependency of a dynamic viscoelasticity thereof (frequency:10 rad/s, −70 to 180° C.), preferably being 0.5 or more, more preferably0.8 or more, still more preferably 1.0 or more. The temperature givingthe maximum value of tan δ is −10 to 40° C., preferably 0 to 40° C.

The copolymer composition having a maximum value of tan δ being withinthis range can exhibit excellent stress absorption and vibration dampingproperties. The maximum value of tan δ can be controlled by comonomercompositional ratio in the copolymer (AA), mixing ratio in the copolymercomposition (Y), and the like. For example, controlling the content of4-methyl-1-pentene so as to be within 10 to 80 wt % can make the maximumvalue of tan δ be within the above range.

The copolymer composition (Y) according to the present invention mayhave various additives blended therein as needed, to the degree notadversely affecting the object of the present invention. With regard tothe additives, the foregoing descriptions can be referred to.

The copolymer composition (Y) according to the present invention maycontain rosin-based resins, terpene-based resins, petroleum resins andthe like, to the degree not adversely affecting the object of thepresent invention. With regard to these resins, the foregoingdescriptions can be referred to.

<Crystalline Olefin Resin (BB)>

The crystalline olefin resin (BB) used in the present invention isemployed without particular limitation as long as being an olefin resinhaving crystallinity and excluding the 4-methyl-1-pentene/α-olefincopolymers (A) to (A3) and the 4-methyl-1-pentene copolymer (AA)according to the present invention. The crystalline olefin as usedherein means a crystalline olefin having a melting point of 100° C. orhigher, preferably 110° C. or higher, and is distinguished from anα-olefin polymer (CC), described later, in terms of a melting point.

The crystalline olefin resin (BB) is particularly a resin havingcrystallinity among the thermoplastic resin (B) as described above.Examples thereof include low-density polyethylene, medium-densitypolyethylene, high-density polyethylene, low-density polyethylene byhigh pressure process, isotactic polypropylene, syndiotacticpolypropylene, poly-1-butene, poly(4-methyl-1-pentene),poly-3-methyl-1-butene, ethylene/α-olefin copolymers, propylene/α-olefincopolymers, and 1-butene/α-olefin copolymers. Preferred examples arepolypropylene, poly(4-methyl-1-pentene), polyethylene and polybutene.

Examples of the polypropylene include an isotactic polypropylene and asyndiotactic polypropylene. The isotactic polypropylene may be ahomopolypropylene, a random copolymer of propylene and an α-olefinhaving 2 to 20 carbon atoms (except for propylene), or a propylene blockcopolymer.

The poly(4-methyl-1-pentene) herein is different from theabove-described copolymer, and examples thereof include a4-methyl-1-pentene homopolymer, a 4-methyl-1-pentene/α-olefin randomcopolymer containing 4-methyl-1-pentene in an amount of 80 to 99.9 wt %,preferably 90 to 99.9 wt % and an α-olefin having 2 to 20 carbon atoms,preferably 6 to 20 carbon atoms, in an amount of 0.1 to 20 wt %,preferably 0.1 to 10 wt %. In the case of the4-methyl-1-pentene/α-olefin random copolymer, examples of the α-olefinto be copolymerized with 4-methyl-1-pentene are those having 2 to 20carbon atoms, preferably 6 to 20 carbon atoms, such as ethylene,propylene, 1-butene, 1-hexene, 1-octene, 1-decene, 1-dodecene,1-tetradecene, 1-hexadecene, 1-octadecene and 1-eicosene. These can beused in a single kind, or can be combined in two or more kinds. Thepoly(4-methyl-1-pentene) desirably has a melt flow rate (MFR; ASTM1238,260° C., 5.0 kg load) of 0.1 to 200 g/10 minutes, preferably 1 to 150g/10 minutes. The poly(4-methyl-1-pentene) may be acommercially-available product, with examples thereof including TPX(trademark) manufactured by Mitsui Chemicals, Inc. Products ofpoly(4-methyl-1-pentene) available from other manufacturers can besuitably used as long as satisfying the above requirement.

Examples of the polyethylene employable include those produced by ahitherto known technique, such as low-density polyethylene,medium-density polyethylene, high-density polyethylene, and low-densitypolyethylene by high pressure process.

The polybutene is a 1-butene homopolymer, or a copolymer of 1-butene andan olefin excluding 1-butene. Examples of the olefin are those describedabove, and these olefins are used in a single kind, or are combined intwo or more kinds. Examples of the copolymer include 1-butene/ethylenerandom copolymer, 1-butene/propylene random copolymer,1-butene/methylpentene copolymer, 1-butene/methylbutene copolymer, and1-butene/propylene/ethylene copolymer. In these copolymers, in terms ofheat resistance, the content of 1-butene is preferably 50 mol % or more,more preferably 70 mol % or more, still more preferably 85 mol % ormore.

The crystalline olefin resin (BB) is not particularly limited, butpreferably has a MFR, as measured in accordance with JIS K-6721, at 190°C. and 230° C., under a load of 2.16 kg, of 0.01 to 150 g/10 minutes,more preferably 0.05 to 100 g/10 minutes, still more preferably 0.1 to100 g/10 minutes, and preferably has a density of 0.990 to 0.800 g/cm³,more preferably 0.980 to 0.810 g/cm³, still more preferably 0.970 to0.830 g/cm³. These ranges are preferred in terms of crystallinity.

Other examples include cyclic olefin copolymers, chlorinatedpolyolefins, vinyl acetate copolymer, ethylene/methacrylate (acrylate)copolymer, ionomers, and ethylene/vinyl alcohol copolymers.

In the present invention, among these resins (BB), a single kind thereofcan be used, or two or more kinds thereof can be combined and used.

Preferred examples of the crystalline olefin resin (BB) according to thepresent invention include polyethylene, polypropylene, poly-1-butene,and poly(4-methyl-1-pentene). More preferred is polypropylene.

<α-Olefin Copolymer (CC)>

The α-olefin copolymer (CC) according to the present invention is notparticularly limited as long as being a copolymer selected fromα-olefins having 2 to 20 carbon atoms and having a melting point oflower than 100° C., provided that the α-olefin copolymer (CC) excludesthe 4-methyl-1-pentene/α-olefin copolymers (A) to (A3) and the4-methyl-1-pentene copolymer (AA) according to the present invention.The melting point is preferably 95° C. or lower, more preferably 90° C.or lower, particularly preferably 85° C. or lower.

Examples of the α-olefin copolymer (CC) include linear α-olefins having2 to 20 carbon atoms, preferably 2 to 15 carbon atoms, more preferably 2to 10 carbon atoms, such as ethylene, propylene, 1-butene, 1-pentene,1-hexene, 1-octene, 1-decene, 1-undecene, 1-dodecene, 1-tetradecene,1-hexadecene, 1-octadecene and 1-eicosene; and more preferred examplesinclude ethylene, propylene, 1-butene, 1-pentene, 1-hexene and 1-octene.Other examples are branched α-olefins preferably having 5 to 20 carbonatoms, more preferably 5 to 15 carbon atoms, such as 3-methyl-1-butene,3-methyl-1-pentene, 3-ethyl-1-pentene, 4-methyl-1-pentene,4,4-dimethyl-1-pentene, 4-methyl-1-hexene, 4,4-dimethyl-1-hexene,4-ethyl-1-hexene, and 3-ethyl-1-hexene.

These α-olefins can be used in a single kind, or can be combined in twoor more kinds.

(d-1): The α-olefin copolymer (CC) comprises, as α-olefins:

a structural unit derived from ethylene, propylene or butene-1 in anamount of 50 to 99 wt %, preferably 50 to 98 wt %, more preferably 50 to95 wt %, and

a structural unit derived from an α-olefin having 2 to 20 carbon atomsother than the above structural unit in an amount of 1 to 50 wt %,preferably 2 to 50 wt %, more preferably 5 to 50 wt %, provided that thetotal amount of the structural units in the copolymer (CC) is 100 wt %.

The inclusion of the α-olefins as described above is preferred in termsof flexibility.

(d-3): The α-olefin copolymer (CC) comprises α-olefins composed of twoor more of ethylene, propylene and butene-1, a structural unit derivedfrom a main component among these three kinds being contained in anamount of 50 to 98 wt %, preferably 50 to 96 wt %, more preferably 50 to95 wt %, provided that the total amount of the structural units in thecopolymer (CC) is 100 wt %.

The inclusion of the α-olefins as described above is preferred in termsof flexibility.

(d-2): The α-olefin copolymer (CC) has a MFR, as measured in accordancewith JIS K-6721, at 190° C. and 230° C., under a load of 2.16 kg, of0.01 to 100 g/10 minutes, more preferably 0.05 to 100 g/10 minutes, andhas a density of 0.910 to 0.850 g/cm³, more preferably 0.900 to 0.860g/cm³. These ranges are preferred in terms of flexibility and mechanicalproperties.

The α-olefin copolymer (CC) usually has an intrinsic viscosity [η], asmeasured in 135° C. decalin, of 0.1 to 10 dL/g, more preferably 0.5 to 5dL/g.

The α-olefin copolymer (CC) may contain, in addition to these units,units derived from other polymerizable monomers, to the degree notadversely affecting the object of the present invention.

Examples of these other polymerizable monomers include:

vinyl compounds such as styrene, vinylcyclopentene, vinylcyclohexane,and vinylnorbornane;

vinyl esters such as vinyl acetate;

unsaturated organic acids such as maleic anhydride, or derivativesthereof;

conjugated dienes such as butadiene, isoprene, pentadiene, and2,3-dimethylbutadiene;

non-conjugated polyenes such as 1,4-hexadiene, 1,6-octadiene,2-methyl-1,5-hexadiene, 6-methyl-1,5-heptadiene, 7-methyl-1,6-octadiene,dicyclopentadiene, cyclohexadiene, dicyclooctadiene, methylenenorbornene, 5-vinylnorbornene, 5-ethylidene-2-norbornene,5-methylene-2-norbornene, 5-isopropylidene-2-norbornene,6-chloromethyl-5-isopropenyl-2-norbornene,2,3-diisopropylidene-5-norbornene,2-ethylidene-3-isopropylidene-5-norbornene, and2-propenyl-2,2-norbornadiene.

The α-olefin copolymer (CC) may contain units derived from these otherpolymerizable monomers in an amount of not more than 10 mol %,preferably not more than 5 mol %, more preferably not more than 3 mol %.

The α-olefin copolymer (CC) is preferably an olefin random copolymer(CC1). Examples of the olefin random copolymer (CC1) includeethylene/propylene random copolymer, ethylene/1-butene random copolymer,ethylene/propylene/1-butene random copolymer,ethylene/4-methyl-1-pentene random copolymer, ethylene/1-hexene randomcopolymer, ethylene/1-octene random copolymer,ethylene/propylene/ethylidenenorbornene random copolymer,ethylene/propylene/vinylidenenorbornene random copolymer,ethylene/1-butene/ethylidenenorbornene random copolymer,ethylene/1-butene/1-octene random copolymer, propylene/1-butene randomcopolymer, butene/4-methyl-1-pentene random copolymer,propylene/1-hexene random copolymer, propylene/1-octene randomcopolymer, butene/1-hexene random copolymer, and butene/1-octene randomcopolymer.

Of these, particularly preferred are ethylene/propylene randomcopolymer, ethylene/1-butene random copolymer,ethylene/propylene/1-butene random copolymer, ethylene/1-butene/1-octenerandom copolymer, ethylene/1-hexene random copolymer, ethylene/1-octenerandom copolymer, propylene/1-butene random copolymer,propylene/1-hexene random copolymer, and propylene/1-octene randomcopolymer.

These copolymers may be used in a single kind, or may be combined in twoor more kinds.

In the present invention, the use of the α-olefin copolymer (CC)improves, in particular, the balance between impact resistance andstress absorption.

The olefin copolymer (CC) can be produced by hitherto known methods,using e.g., a vanadium catalyst, a titanium catalyst or a metallocenecatalyst. The olefin copolymer (CC) may be a commercially-availableproduct, with examples including a product named “TAFMER™” manufacturedby Mitsui Chemicals, Inc.

<Production Method of Copolymer Composition>

Methods for producing the 4-methyl-1-pentene/α-olefin copolymercompositions (X) to (X22) and the 4-methyl-1-pentene/α-olefin copolymercomposition (Y) of the present invention are described.

The copolymer composition can be produced using the individualcomponents in the above ranges, by various known processes using, forexample, multistep polymerization method, a mixing method using aPlastomill, a Henschel mixer, a V-blender, a ribbon blender, a tumblerblender, a kneader ruder or the like, or a method comprising mixing,melt-kneading using a single-screw extruder, a twin-screw extruder, akneader, a Banbury mixer or the like, and granulation or pulverization.

<Articles>

Articles comprising the 4-methyl-1-pentene/α-olefin copolymer accordingto the present invention, articles comprising the4-methyl-1-pentene/α-olefin copolymer composition according to thepresent invention, and articles comprising the 4-methyl-1-pentenecopolymer composition, or articles comprising modified productsobtainable using any of these, are obtainable by known heat moldingmethods such as extrusion molding, injection molding, inflation molding,blow molding, extrusion blow molding, injection blow molding, pressmolding, stamping molding, vacuum molding, calendar molding, filamentmolding, foam molding, and powder slush molding. The articles of thepresent invention can be produced also from an arbitral combination ofthe copolymer, the copolymer composition, according to the presentinvention and modified products thereof.

Hereinafter, the articles are specifically described.

It is also preferable for the articles to be those which are obtained byprimary molding, such as extrusion molding, injection molding andsolution casting, and processed by a method such as blow molding andstretching. For example, it is also preferable for the articles in theform of films or sheets to be those obtained by subjecting articles inthe form of sheets obtained by T-die extrusion molding or the like tomonoaxial stretching or biaxial stretching. Among the above uses, usesas films, in which the high melting point property can be takenadvantage of, are preferred.

When performing extrusion molding, hitherto known extrusion apparatusesand molding conditions are adoptable. For example, using a single-screwextruder, a kneading extruder, a ram extruder or a gear extruder, amolten copolymer or composition is extruded from a specific die, wherebythe copolymer or composition can be molded to have a desired form.

Stretched films are obtainable by stretching such extruded sheets orextruded films (unstretched) as mentioned above by a known stretchingmethod, such as tentering (lengthwise-crosswise stretching,crosswise-lengthwise stretching), simultaneous biaxial stretching andmonoaxial stretching.

In stretching sheets or unstretched films, the stretching ratio isusually about 20 to 70 times for biaxial stretching, and is usuallyabout 2 to 10 times for monoaxial stretching. It is desirable thatstretching provides a stretched film having a thickness of about 5 to200 μm.

Furthermore, as articles in the form of films, inflation films can beproduced. Inflation molding is unlikely to cause drawdown.

Blow molded articles can be produced using hitherto known blow moldingapparatus under known conditions. In this case, the resultant blowmolded article may be a multilayer article, which has at least one layercomposed of the copolymer or copolymer composition according to thepresent invention or a modified product thereof.

In extrusion blow molding, for example, a resin at a molten state isextruded from a die at a resin temperature of 100° C. to 300° C. to forma tubular parison, and the parison is held in a mold with a desiredshape, to which air is blown, and the parison is fitted to the mold at aresin temperature of 130° C. to 300° C., whereby a hollow article can beproduced. The stretching (blowing) ratio is desirably about 1.5 to 5times in crosswise direction.

In injection blow molding, a resin is injected into a parison mold at aresin temperature of 100° C. to 300° C. to form a parison, and theparison is held in a mold with a desired shape, to which air is blown,and the parison is fitted to the mold at a resin temperature of 120° C.to 300° C., whereby a hollow article can be produced. The stretching(blowing) ratio is desirably 1.1 to 1.8 in lengthwise direction and 1.3to 2.5 times in crosswise direction.

The resultant blow molded articles are excellent in transparency,rigidity or flexibility, heat resistance, and impact resistance, andfurther in moisture resistance.

As pressed articles, mold stamping articles can be mentioned. The moldstamping articles are obtainable, for example, by a method in which asubstrate and a skin material are simultaneously subjected to pressmolding thereby subjecting the two to composite integral molding (moldstamping molding). The substrate can be formed from the copolymer orcopolymer composition according to the present invention or modifiedproducts thereof. The pressed articles are hardly electrostaticallycharged and are excellent in rigidity or flexibility, heat resistance,transparency, impact resistance, aging resistance, surface gloss,chemical resistance, abrasion resistance, etc.

Foamed articles comprising the copolymer or copolymer compositionaccording to the present invention or modified products thereof areobtainable at a high foaming ratio, and have good injection moldability,and high rigidity and material strength.

Filament articles can be produced by, for example, extruding a moltencopolymer or copolymer composition, or modified products thereof througha spinneret. Specifically, spunbond method or meltblown method ispreferably employed. The filament thus obtained may be furtherstretched. The stretching is sufficient as long as being performed tosuch an extent that in at least monoaxial direction of the filament,molecules become oriented. The desirable stretching ratio is usuallyabout 5 to 10 times. The filament articles according to the presentinvention are hardly electrostatically charged and are excellent intransparency, flexibility, heat resistance, impact resistance andstretchability.

From the articles of the present invention, it is possible to producepowder slush articles such as automotive parts, household electricalappliance parts, toys, and sundries. Such articles are hardlyelectrostatically charged and are excellent in flexibility, heatresistance, aging resistance, surface gloss, chemical resistance,abrasion resistance, etc.

A further example of the articles of the present invention is a laminatehaving at least one layer composed of the copolymer or copolymercomposition according to the present invention or modified productsthereof. Such a laminate is excellent in vibration damping properties,e.g., impact reduction and shock relaxation, and impact absorption.

In the case of uses as additive materials, the materials are obtained bya method in which during molding the thermoplastic resins ((B), (BB) and(CC)) according to the present invention, the copolymer according to thepresent invention is added (for example, the thermoplastic resins aremolded in a molding machine (extruder), and in the middle of the molding(extrusion), the copolymer is fed). The thermoplastic resins are moldedin a molten state by a method that involves at least one of shear flow,monoaxial flow, biaxial flow and planar elongational flow; as such amethod, a known method is adoptable without particular limitation. Themolding methods involving shear flow are, for example, extrusionmolding, injection molding and melt blow molding. The molding methodsinvolving monoaxial flow, biaxial flow or planar elongational flow are,for example, known methods such as T-die (film) molding, blow moldingand stretching. The molten state as used herein refers to a range thatis from not lower than a melting point of the copolymer or copolymercomposition of the present invention or modified products thereof toless than 350° C., preferably from 170° C. to 350° C.

The 4-methyl-1-pentene/α-olefin copolymers ((A) to (A3)) according tothe present invention are thermodynamically incompatible withthermoplastic resins. It is thus considered that the4-methyl-1-pentene/α-olefin copolymers are localized on surfaces of thearticles thus obtained.

<Uses>

Uses of the 4-methyl-1-pentene/α-olefin copolymers (A to A3), the4-methyl-1-pentene/α-olefin copolymer compositions (X to X22), and the4-methyl-1-pentene copolymer composition (Y) according to the presentinvention, or graft modified products and crosslinked products thereofare described.

(1) The 4-methyl-1-pentene/α-olefin copolymer (A) is excellent intransparency, impact resistance, heat resistance, lightness, flexibilityor rigidity, stress absorption, stress relaxation, scratch resistance,abrasion resistance, mechanical properties, toughness, soundproofproperty, vibration damping properties, cutting property, high breakdownvoltage, gas permeability, shrinkability, rubber elasticity, kinkresistance, stretchability, creep characteristics, adhesion, surfacetension, flexibility modification property, transparency modificationproperty, no stickiness in molding operation, etc., and therefore can beused favorably for the following uses.

As articles comprising the copolymer composition according to thepresent invention, examples are sheets, films, pipes, tubes, bottles,fibers, tapes, hollow articles, laminates and foamed products.

As a resin excellent in transparency, gas permeability, chemicalresistance and peeling property, and in releasability and heatresistance, the copolymer according to the present invention are used invarious fields including medical equipment, heat resistant wires, heatresistant eating utensils and peeling materials.

The articles as sheets and films are hardly electrostatically chargedand are excellent in mechanical properties, heat resistance,stretchability, impact resistance, aging resistance, transparency,see-through property, gloss, rigidity, moisture resistance, and gasbarrier property, and can be used as soundproof sheets,vibration-damping sheets, heat-shielding sheets, heat-shielding films,packaging films, food packaging films (outer layers, inner layers,sealants and single layers), stretchable films, plastic wraps, stretchedfilms, air-breathable films, shrink films, etc.

The injection molded articles are hardly electrostatically charged andare excellent in transparency, rigidity, heat resistance, impactresistance, surface gloss, chemical resistance, abrasion resistance,etc., and can be widely used as automotive interior trims, automotiveexterior trims, housings for household electrical appliances,containers, etc.

The mold stamping articles can be used as automotive interior trims,such as door trims, rear package trims, seat back garnishes andinstrument panels.

The vacuum articles can be used as interior skin materials, such asinstrument panels and door trims. Such molded products are hardlyelectrostatically charged and are excellent in flexibility, heatresistance, impact resistance, aging resistance, surface gloss, chemicalresistance, abrasion resistance, etc.

Exemplary uses of the articles comprising the copolymer according to thepresent invention are described hereinafter, without particularlylimiting thereto.

As containers, examples include food containers, retort containers andbottles, e.g., eating utensils, retort containers, freeze preservationcontainers, retort pouches, microwave oven heat-resistant containers,frozen food containers, chilled sweet cups, cups and beverage bottles;blood transfusion sets, medical bottles, medical containers, medicalhollow bottles, medical bags, transfusion bags, blood preservation bags,transfusion bottle chemicals containers, detergent containers, cosmeticscontainers, perfume containers, and toner containers.

As modifiers, examples include resin modifiers, compatibilizers (graftmodification) and easy-peeling properties modifiers, e.g., polypropylenemodifiers, poly(4-methyl-1-pentene) modifiers, polybutene modifiers,polyethylene modifiers, styrene elastomer modifiers, butyl rubbermodifiers, propylene elastomer modifiers, ethylene elastomer modifiers,modifiers for acrylic adhesives, hot melt adhesive modifiers, flow markmodifiers, weld modifiers, surface modifiers and gas barrier modifiers.

As packaging materials, examples include food packaging materials, meatpackaging materials, processed fish packaging materials, vegetablepackaging materials, fruit packaging materials, fermented food packagingmaterials, sweets packaging materials, oxygen-absorbent packagingmaterials, packaging materials for retort food, freshness preservationfilms, drug packaging materials, cell culture bags, cell inspectionfilms, bulb packaging materials, seed packaging materials, films forvegetables/fungus cultivation, heat-resistant vacuum molded containers,prepared food containers, lids for prepared food, industrial plasticwraps, household plastic wraps, and baking cartons.

As films, sheets and tapes, examples include:

releasing films for flexible print substrates, releasing films for rigidsubstrates, releasing films for rigid flexible substrates, releasingfilms for advanced composite materials, releasing films for the curingof carbon fiber composite materials, releasing films for the curing ofglass fiber composite materials, releasing films for the curing ofaramid fiber composite materials, releasing films for the curing of nanocomposite materials, releasing films for the curing of fillers,releasing films for sealing semiconductors, releasing films forpolarizing plates, releasing films for diffusion sheets, releasing filmsfor prism sheets, releasing films for reflection sheets, cushion filmsfor releasing films, releasing films for fuel batteries, releasing filmsfor various rubber sheets, releasing films for the curing of urethane,and releasing films for the curing of epoxy;

solar battery cell sealing sheets, solar battery cell back sheets,plastic films for solar batteries, battery separators, separators forlithium ion batteries, electrolyte membranes for fuel batteries, andadhesive/pressure-sensitive adhesive separators;

substrates, adhesives and separators for semiconductor process filmssuch as dicing tapes, back grind tapes, die bonding films, two-layerFCCL and films for film capacitors; adhesive films, films for pellicles;films for polarizing plates; protecting films such as polarizing plateprotecting films, liquid crystal panel protecting films, opticalcomponent protecting films, lens protecting films, electriccomponent/electric appliance protecting films, mobile phone protectingfilms, personal computer protecting films, masking films, films forcapacitors, reflection films, laminates (including glass), radiationresistant films, γ-ray resistant films, and porous films;

heat dissipation films/sheets, flasks for the production of electroniccomponent sealants, LED molds, laminate plates for high-frequencycircuits, high-frequency cable coating materials, optical waveguidesubstrates;

glass interlayers, films for safety glass, bulletproof materials, filmsfor bulletproof glass;

releasing paper such as releasing paper for synthetic leather, releasingpaper for advanced composite materials, releasing paper for the curingof carbon fiber composite materials, releasing paper for the curing ofglass fiber composite materials, releasing paper for the curing ofaramid fiber composite materials, releasing paper for the curing of nanocomposite materials, and releasing paper for the curing of fillers; andheat-resistant water resistant printing paper.

As other uses, examples include mandrels for the production of rubberhoses, sheaths, sheaths for the production of rubber hoses, hoses,tubes, wire coating materials, insulators for high-voltage wires, wiringducts, tubes for cosmetics and perfume sprays, medical tubes,transfusion tubes, pipes and wire harness;

interior trims of automobiles, motorcycles, railroad vehicles, airplanes, ships, etc.; abrasion-resistant automotive interior and exteriortrims; automotive interior and exterior trims such as instrument panelskins, door trim skins, rear package trim skins, ceiling skins, rearpillar skins, seatback garnishes, console boxes, arm rests, air backcase lids, shift knobs, assist grips, side step mats, reclining covers,sheets in trunks, seatbelt buckles, moldings such as inner/outermoldings, roof moldings, and belt moldings, automotive seal materialssuch as door seals and body seals, glass run channels, mudguards,kicking plates, step mats, number plate housings, automotive hosecomponents, air duct hoses, air duct covers, air intake pipes, air damskirts, timing belt cover seals, hood cushions, and door cushions;special tires such as vibration damping tires, silent tires, car racetires, and radio control tires; packings, automotive dust covers, lampseals, automotive boots, rack and pinion boots, timing belts, wireharness, grommets, emblems, air filter packings;

skin materials of e.g., furniture, shoes, cloths, bags and buildingmaterials, seal materials for architecture, waterproof sheets, buildingmaterial sheets, building material gaskets, window frames for buildingmaterials, iron-core protecting components, gaskets, doors, door frames,window frames, cornices, baseboards, opening frames, floor materials,ceiling materials, wall paper;

health appliances (e.g., nonslip mats/sheets and tip-resistantfilms/mats/sheets), health appliance components, impact absorbing pads,protectors/protecting components (e.g., helmets and guards), sport gears(e.g., sport grips and protectors), sport protecting equipment, rackets,mouth guards, balls, golf balls; carrying implements (e.g., impactabsorbing grips for carrying and impact absorbing sheets); impactabsorbers such as vibration damping pallets, impact absorbing dampers,insulators, impact absorbers for shoes, impact absorbing foamedproducts, and impact absorbing films;

grips, sundries, toys, treads, shoe soles, shoe midsoles/inner soles,soles, sandals, suckers, tooth blushes, floor materials, gymnastic mats,electrical tool components, agricultural equipment components, heatdissipation materials, transparent substrates, soundproof materials,cushion materials, wire cables, shape memory materials;

medical gaskets, medical caps, drug caps, gaskets; packing materialsused in high-temperature treatments such as boiling treatment andhigh-pressure steam sterilization carried out after filling bottles withbaby food, dairy products, drugs, sterilized water and the like;industrial seal materials, industrial sewing machine tables, numberplate housings, cap liners such as PET bottle cap liners;

adhesives such as protecting film adhesive layers and hot meltadhesives;

stationery, office supplies; supports of precision devices and officeautomation devices such as office automation printer legs, facsimilelegs, sewing machine legs, motor supporting mats and audiovibration-proof materials; heat-resistant packings for officeautomation, animal cages, physical and chemical science experimentalequipment such as beakers and measuring cylinders, cells for opticalmeasurement, cloth cases, clear cases, clear files, clear sheets, deskmats;

uses as fibers such as nonwoven fabrics, stretchable nonwoven fabrics,fibers, waterproof fabrics, air-breathable woven fabrics and fabrics,disposable diapers, sanitary products, hygiene products, filters, bugfilters, dust-collecting filters, air cleaners, hollow fiber filters,water-purifying filters, filter fabrics, filter paper, and gasseparation membranes.

Further preferred uses include coating materials, films and sheetsobtained by coating, water repellants, insulating films, pressuresensitive adhesives, adhesives, coated paper, transparent sealants,sealants, hot melt type adhesives/pressure sensitive adhesives, solventtype adhesives/pressure sensitive adhesives, film-likeadhesives/pressure sensitive adhesives, fabric tapes, craft tapes, andelastomeric pressure-sensitive adhesives.

The copolymer and the composition are favorably used particularly in thefields (1) to (3) as described below, which take advantage of thecharacteristics of the present invention.

[(1) Films]

Uses to take advantage of the releasability of films and sheets arepreferred. A specific example is an adhesive film in which a knownadhesive layer is formed on a film. Examples of the adhesive layerinclude acrylic adhesive layers, ester adhesive layers, olefin adhesivelayers, and urethane adhesive layers. As these adhesive layers,materials having adhesive power appropriate for corresponding substratesare employable.

In addition to these, further examples are polarizing plate protectingfilms or FPD (flat panel display) protecting films with a multilayerfilm structure comprising a film for protecting a polarizing plate, FPDor the like, an adhesive layer and the 4-methyl-1-pentene/α-olefincopolymer film. Specific examples are those described as the protectingfilms. Still further examples include easy-peeling properties modifiers,releasing materials, and uses in packaging materials to take advantageof the heat resistance and mechanical properties etc., which usesinclude packaging films and sheets, films (outer layers, inner layers,sealants, single layers) for food packaging, stretchable films, plasticwraps, stretched films, air-breathable films, shrink films, microwaveoven heat resistant containers, frozen food containers, meat packagingmaterials, processed fish packaging materials, vegetable packagingmaterials, fruit packaging materials, fermented food packagingmaterials, sweets packaging materials, oxygen-absorbent packagingmaterials, packaging materials for retort food, freshness preservationfilms, drug packaging materials, cell culture bags, cell inspectionfilms, bulb packaging materials, seed packaging materials, films forvegetables/fungus cultivation, heat-resistant vacuum molded containers,prepared food containers, lids for prepared food, industrial plasticwraps, and household plastic wraps.

As specific examples, the above-mentioned releasing films can bementioned.

In the case of the packaging films, the articles obtained as films andsheets may be multilayer articles. Examples of the multilayer articlesinclude the above substrates, adhesives and separators for semiconductorprocess films, adhesive films, films for pellicles, films for polarizingplates, the above protecting films, and heat dissipation films/sheets.

[(2) Vibration Damper]

The copolymer and copolymer composition according to the presentinvention are suited for stress absorbers/vibration dampers excellent instress absorption and vibration damping properties, and articlesthereof, and in detail, suited for stress absorbers/vibration dampersfor non-vinyl-chloride polymer materials having good mechanicalproperties (breaking strength and tensile modulus). Specific examplesinclude office automation devices, household electrical appliances suchas washing machines, automobiles, machine tools, industrial machines,floor materials, vibration damping panels and vibration dampingarticles.

The copolymer and copolymer composition according to the presentinvention and modified products thereof, having a high peak value of tanδ, are suited as stress absorbers/vibration dampers. In particular, the4-methyl-1-pentene/α-olefin copolymer is preferably a copolymer of4-methyl-1-pentene and an α-olefin having 2 to 4 carbon atoms. Thecopolymer of 4-methyl-1-pentene and an α-olefin having 2 to 4 carbonatoms may contain a non-conjugated polyene.

The copolymer according to the present invention or modified productsthereof may have thermoplastic resins added thereto, as needed. Thethermoplastic resin herein is, for example, the above-describedthermoplastic resin (B). Preferred examples include:

olefin polymers such as polyethylene, polypropylene, and copolymers ofethylene and/or propylene and an α-olefin, excluding the copolymeraccording to the present invention; and styrene polymers such aspolystyrene, high-impact polystyrene, styrene/methacrylic acid estercopolymers (MS), acrylonitrile/styrene copolymer (AS),acrylonitrile/butadiene/styrene copolymer (ABS),styrene/isoprene/styrene copolymer (SIS) and hydrogenated productsthereof, styrene/butadiene/styrene copolymer (SBB) and hydrogenatedproducts thereof, and styrene/isobutylene/styrene copolymer (SIBS) andhydrogenated products thereof. These resins are preferred in terms ofcompatibility, moldability and the like.

These thermoplastic resins can be used in a single kind, or can becombined in two or more kinds.

A molecular weight of the thermoplastic resin is not particularlylimited, but a weight-average molecular weight in terms of polystyreneis preferably 5,000 to 1,000,000, more preferably 50,000 to 500,000.This range achieves the characteristics of the present invention,moldability, and the like with good balance.

The thermoplastic resin is added usually in an amount of 0 to 99 wt %,more preferably 0 to 95 wt %, still more preferably 0 to 90 wt %, basedon 100 wt % of the total of the copolymer and the thermoplastic resin.If the addition amount is more than 99 wt %, the effects of thecopolymer (A), for example, properties such as stressabsorption/vibration damping properties, mechanical properties, heatresistance, and chemical resistance, cannot be exhibited. The copolymer,in order to exhibit its vibration damping properties and the like, isused preferably in an amount of 5 to 100 wt %, more preferably 10 to 100wt %, based on 100 wt % of the total of the copolymer and thethermoplastic resin.

The stress absorber/vibration damper can have inorganic fillers addedthereto, as needed. Examples of the inorganic fillers include mica(scale-form, i.e., flaky mica or the like), talc, clay, calciumcarbonate, aluminum hydroxide, hydrotalcite, glass fibers, glass bead,glass balloon, glass flake, silica, carbon black, graphite, titaniumoxide, magnesium hydroxide, potassium titanate whisker, and carbonfibers, with forms thereof being not particularly limited and includingscale form, spherical form, granular form, powder form and amorphousform. The addition of the inorganic fillers can improve mechanicalproperties such as vibration damping properties and modulus ofelasticity, dimensional stability, and chemical resistance; however, thefluidity may be lowered. These inorganic fillers are added in an amountof 0 to 100 parts by weight, preferably 0 to 70 parts by weight, morepreferably 0 to 40 parts by weight, based on 100 parts by weight of thetotal of the polymer according to the present invention and thethermoplastic resin (B).

The stress absorber/vibration damper of the present invention can havevarious additives added thereto, as needed. With regard to theadditives, the foregoing descriptions can be referred to.

The stress absorber/vibration damper of the present invention has amaximum value of loss tangent tan δ of kinematic viscoelasticity, asmeasured within a temperature range of −70 to 180° C. at a frequency of10 rad/s, of 0.1 to 10. Preferably, the temperature giving the peakvalue ranges from −50 to 100° C., more preferably from −40 to 50° C.,still more preferably from −30 to 50° C., most preferably from −10 to40° C. The maximum value of the tan δ is preferably 0.4 to 8,particularly preferably 0.6 to 6, more preferably 0.7 to 5. The maximumvalue of tan δ within these ranges can give excellent stress absorptionand vibration damping properties. The maximum value as used herein isdetermined based on sufficiently averaged data in terms of dispersionand the like of the measurement.

The stress absorber/vibration damper of the present invention has anextremely high peak value of loss coefficient tan δ of kinematicviscoelasticity, at around room temperature, and furthermore has goodmechanical properties (breaking strength and tensile modulus), chemicalresistance and stress absorption. The stress absorber/vibration damperof the present invention is suited as vibration dampers, soundproofmaterials or sound insulators in e.g., office automation devices,industrial machines, automobiles, railroads, bridges, ships, buildingmaterials, interior materials, audio devices and household electricalappliances such as air conditioners and washing machines.

[(3) Additive Material]

The copolymer or copolymer composition of the present invention, becauseof having excellent anti-blocking effect and releasability, is suited asan additive material.

After the copolymer or copolymer composition according to the presentinvention or a modified product thereof is blended with a thermoplasticresin or a thermosetting resin to form a thermoplastic resin compositionor a thermosetting resin composition, the composition is used inarticles such as films, bottles and cases, and can give excellentreleasability and water repellency to such articles. Moreover, thecomposition can give excellent releasability from molds in injectionmolding. The copolymer, the copolymer composition or a modified productthereof hardly bleed-outs with the passage of time, and moreover doesnot cause odor or smoke. Furthermore, the 4-methyl-1-pentene/α-olefincopolymer, because of having a transparent skeleton, is considered tohardly deteriorate the transparency of articles.

If propylene resins are blended with the additive materials, theresultant articles are provided with excellent transparency, scratchresistance, whitening resistance and heat resistance attributable to thepropylene resins, and do not have stickiness even when used at hightemperature, and therefore such articles are employable under conditionswith a wide temperature range.

In uses of the present invention as the additive materials, inparticular, the copolymer, the copolymer composition and modifiedproducts thereof preferably have a small molecular weight, a narrowmolecular weight distribution, and less content in low-molecular regionof the molecular weight distribution. The 4-methyl-1-pentene/α-olefincopolymer is preferably a copolymer of 4-methyl-1-pentene and anα-olefin having 2 to 3 carbon atoms. The copolymer of 4-methyl-1-penteneand an α-olefin having 2 to 3 carbon atoms may contain a non-conjugatedpolyene. In uses as additive material, the copolymer, the copolymercomposition, or a modified product thereof is used in an amount of 0.01to 10 parts by weight, preferably 0.1 to 7 parts by weight, morepreferably 0.2 to 5 parts by weight, based on 100 parts by weight ofthermoplastic resins. The thermoplastic resins herein are notparticularly limited, but the above-described thermoplastic resin (B)can be mentioned as an example. The thermoplastic resins can be used ina single kind, or can be combined in two or more kinds.

(2) The 4-methyl-1-pentene/α-olefin copolymer (A1) according to thepresent invention is excellent in transparency, stress absorption,impact resistance, lightness, flexibility, stress relaxation, soundproofproperty, vibration damping properties, cutting property, high breakdownvoltage, gas permeability, shrinkability, rubber elasticity, kinkresistance, adhesion, flexibility modification property, andtransparency modification property, and therefore can be used favorablyfor the above-described uses. The copolymer (A1) according to thepresent invention can be favorably used particularly for vibrationdampers, vibration-proof materials, soundproof materials or soundinsulators in e.g., office automation devices, industrial machines,automobiles, railroads, bridges, ships, building materials such asvibration damping mats and vibration dampers, interior materials, audiodevices and household electrical appliances such as air conditioners andwashing machines; impact absorbers such as mouth guards, sportprotectors, protectors for nursing care and impact absorbing mats;adhesives such as adhesive films and protecting film adhesive layers;protecting films; and modifiers such as polyolefin modifiers, elastomermodifiers, hot melt adhesive modifiers, and easy-peeling propertiesmodifiers.

(3) The 4-methyl-1-pentene/α-olefin copolymer (A2) according to thepresent invention is suited, among the above-described uses, forvibration dampers, vibration-proof materials, soundproof materials orsound insulators in e.g., office automation devices, industrialmachines, automobiles, railroads, bridges, ships, building materialssuch as vibration damping mats and vibration dampers, interiormaterials, audio devices and household electrical appliances such as airconditioners and washing machines; impact absorbers such as mouthguards, sport protectors, protectors for nursing care, impact absorbingmats and shoe inner soles; adhesives such as adhesive films andprotecting film adhesive layers; protecting films for semiconductorprocess; grips of e.g., spots gears, stationery and health goods; andmodifiers such as polyolefin modifiers, elastomer modifiers, hot meltadhesive modifiers, and easy-peeling properties modifiers.

(4) The 4-methyl-1-pentene/α-olefin copolymer (A3) according to thepresent invention and crosslinked products thereof are, as a resinexcellent in rubber elasticity, compression stress relaxation, heatresistance, foaming property and foaming property modification property,suited particularly for vibration dampers, vibration-proof materials,soundproof materials or sound insulators in e.g., office automationdevices, industrial machines, automobiles, railroads, bridges, ships,building materials such as vibration damping mats and vibration dampers,interior materials, audio devices, and household electrical appliancessuch as air conditioners and washing machines, impact absorbers, grips,vibration damping rubbers, polyolefin modifiers, elastomer modifiers andfoaming modifiers.

(5) The 4-methyl-1-pentene/α-olefin copolymer composition (X) accordingto the present invention is excellent in transparency, stressabsorption, impact resistance, heat resistance, lightness, flexibility,stress relaxation, scratch resistance, abrasion resistance, soundproofproperty, vibration damping properties, cutting property, high breakdownvoltage, gas permeability, shrinkability, rubber elasticity, kinkresistance, adhesion, surface tension, flexibility modificationproperty, and transparency modification property, and therefore can beused favorably for the above-described uses.

(6) The 4-methyl-1-pentene/α-olefin copolymer compositions (X11, X12)according to the present invention can be favorably used for vibrationdampers, vibration-proof materials, soundproof materials or soundinsulators in e.g., office automation devices, industrial machines,automobiles, railroads, ships, building materials such as vibrationdamping mats and vibration dampers, interior materials, audio devicesand household electrical appliances such as air conditioners and washingmachines; violation damping steel plate; impact absorbers such as mouthguards, sport protectors, protectors for nursing care, and impactabsorbing mats; adhesives such as adhesive films and protecting filmadhesive layers; films and sheets such as vibration damping sheets,surface protecting films and protecting films for semiconductor process;and modifiers such as polyolefin modifiers, elastomer modifiers, hotmelt adhesive modifiers, easy-peeling properties modifiers and foamingmodifiers.

(7) The 4-methyl-1-pentene/α-olefin copolymer compositions (X12, X22)according to the present invention can be favorably used forpolypropylene modifiers, poly(4-methyl-1-pentene) modifiers, flexibilitymodifiers, transparency modifiers, grips, packaging films,air-breathable films, medical tubes, industrial tubes, food containers,heat resistant containers, medical containers, animal cages, physicaland chemical science experimental equipment, nonwoven fabrics, andreleasing films.

(8) Uses of the 4-methyl-1-pentene copolymer composition (Y) of thepresent invention are described. The 4-methyl-1-pentene copolymercomposition (Y) is excellent in lightness, flexibility or rigidity,vibration damping properties, stress absorption, stress relaxation,impact resistance, mechanical properties, toughness, soundproofproperty, cutting property, high breakdown voltage, gas permeability,kink resistance, cold resistance, stretchability, creep characteristics,adhesion, flexibility modification property, and has no stickiness inmolding operation, etc., and therefore can be used favorably for theabove-described uses.

EXAMPLES

The present invention is described with reference to Examples, but thepresent invention is in no way limited by these Examples. In the presentinvention, individual properties were measured by the methods asdescribed below.

[Intrinsic Viscosity [η]]

An intrinsic viscosity was measured using a decalin solvent at 135° C.

[Composition and B Value]

¹³C-NMR was employed to measure a content of 4-methyl-1-pentene and acontent of an α-olefin, and an amount of a non-conjugated polyene in apolymer.

The measurement was carried out using ECP 500 nuclear magnetic resonanceapparatus manufactured by JEOL Ltd. As a solvent, a mixed solvent oforthodichlorobenzene/deuterated benzene (80/20 volume %) was used. Thespecimen concentration was 55 mg/0.6 mL, and the measurement temperaturewas 120° C. The observation nucleus was 13C (125 MHz). The sequence wassingle pulse proton decoupling. The pulse width was 4.7 μsec (450pulse). The repeating time was 5.5 sec. The number of integration wasnot lower than 10000. The standard value of chemical shift was definedas 27.50 ppm.

Based on 1³C-NMR spectrum, a B value was calculated from the followingformula using a peak intensity of propylene main chain aa methine I_(P)(2.87 ppm), a peak intensity of 4-methyl-1-pentene main chain αα methineI_(PM) (31.8 ppm) and a peak intensity of main chain aa methylene I_(M)(44.5 ppm).

(B  value) = {I_(PM)/(2 × I_(P)× I_(M))}

[Melting Point (Tm)]

A melting point (Tm) of a polymer was measured by Differential ScanningCalorimetry (DSC) using DSC 220C apparatus manufactured by SeikoInstruments Inc. A specimen obtained by polymerization, weighting 7 to12 mg, was sealed in an aluminum pan, and the specimen was heated at arate of 10° C./min from room temperature to 200° C. For completemelting, the specimen was held at 200° C. for 5 minutes, and then cooledto −50° C. at a rate of 10° C./min. The specimen was allowed to stand at−50° C. for 5 minutes, and then heated for the second time at a rate of10° C./min to 200° C. A peak temperature in this second heating test wasdefined as a melting point (Tm).

[Molecular Weight (Mw, Mn), Molecular Weight Distribution (Mw/Mn)]

A molecular weight of a polymer was measured using a liquidchromatograph (ALC/GPC 150-C plus, manufactured by Waters, differentialrefractive index meter and detector integrated type) As a column, twopieces of GMH6-HT and two pieces of GMH6-HTL, manufactured by TosohCorporation, were connected in series. As a mobile phase medium,o-dichlorobenzene was used. The measurement was carried out at aflowrate of 1.0 mL/min at 140° C. A chromatogram obtained was analyzedby known method, using a calibration that employed a standardpolystyrene sample. Thereby, Mw, Mn and Mw/Mn were calculated.

[Extracted Amount Under Methyl Acetate]

A polymer was collected in a Soxhlet extractor, and was heat refluxedunder methyl acetate. An amount of the polymer was weighed before andafter refluxing and thereby an extracted amount (wt %) was calculated.

[Preparation of Press Sheet for Various Measurements]

Using a hydraulic heat pressing machine manufactured by Shindo KinzokuCo., Ltd., which was set at 200° C., at a pressure of 10 MPa, a sheetwas formed. In the case of a sheet with a thickness of 0.5 to 3 mm (fourspacers were provided on a plate of 240×240×2 mm in thickness; eachspacer had a size of 80×80×0.5 to 3 mm in thickness), preheating wascarried out for about 5 to 7 minutes, and then pressurization wascarried out at 10 MPa for 1 to 2 minutes. Then, using another hydraulicheat pressing machine manufactured by Shindo Kinzoku Co., Ltd., whichwas set at 20° C., compression was carried out at 10 MPa, which wasfollowed by cooling for about 5 minutes. Thereby, a specimen formeasurement was prepared. As a heating plate, a brass plate with athickness of 5 mm was used. The sample obtained was used for theevaluation of various properties.

[Shore Hardness Measurement]

In accordance with JIS K6253, using a press sheet with a thickness of 3mm, measurement was carried out with a shore hardness meter. As a shorehardness meter, an A hardness meter or a D hardness meter was used.Furthermore, a change ΔHS between a value obtained immediately after themeasurement and a value obtained 15 seconds after the measurement wascalculated in the following manner.

ΔHS=(Shore A hardness value measured immediately after the starting ofindenter contact−Shore A hardness value measured 15 seconds after thestarting of indenter contact)

ΔHS=(Shore D hardness value measured immediately after the starting ofindenter contact−Shore D hardness value measured 15 seconds after thestarting of indenter contact)

[Kinematic Viscoelasticity]

A press sheet with a thickness of 3 mm was prepared, from which a striphaving a size of 45 mm×10 mm×3 mm was cut out for kinematicviscoelasticity measurement. The temperature dependency of the kinematicviscoelasticity from −70 to 180° C. at a frequency of 10 rad/s wasmeasured, using MCR301 manufactured by ANTONPaar, and then a peaktemperature giving a peak value of a loss tangent (tan δ) attributed toa glass transition temperature, and the peak value were measured.

[Abrasion Resistance Evaluation]

An abrasion resistance was evaluated based on a percentage of change ingloss (%) obtained by abrasion using Gakushin-type rubbing tester.

Using a Gakushin-type rubbing tester (manufactured by Toyo SeikiSeisaku-Sho, Ltd.), a press sheet with a thickness of 2 mm was abradedwith a 45R abrasion indenter of 1000 g made of SUS, the tip of which hadbeen covered with a cotton canvas of #10, at 23° C., at a reciprocationfrequency of 100 times, at a reciprocation rate of 33 times/min, at astroke of 100 mm. A percentage of change in gloss between before theabrasion and after the abrasion was calculated in the following manner.

ΔG={(gloss before abrasion−gloss after abrasion)/gloss beforeabrasion}×100

[Tensile Modulus (YM), Tensile Elongation at Break (EL), Tensile Stressat Yield (YS), Tensile Stress at Break (TS)]

As tensile properties, a tensile modulus (YM), a tensile elongation atbreak (EL), a tensile stress at yield (YS), a tensile stress at break(TS) were evaluated using half of a No. 2 specimen defined in JIS K7113that was stamped from a press sheet with a thickness of 1 mm obtained bythe above method, at a tensile rate of 30 mm/min under an atmosphere of23° C.

[Tensile Permanent Set (PS)]

A tensile permanent set (PS) was evaluated in the following manner. Halfof a No. 2 specimen defined in JIS K7113 that was stamped from a presssheet with a thickness of 1 mm obtained by the above method was used asa specimen for evaluation. When the specimen had an elongation rate of100% at a tensile rate of 30 mm/min, a distance between chucks at thistime was measured. The specimen was held under an atmosphere of 23° C.for 10 minutes and then released. At 10 minutes past the release, adistance between chucks was measured. A difference between the distanceswas calculated.

[Softening Temperature Based on TMA Measurement]

In accordance with JIS K7196, using a specimen with a thickness of 1 mm,measurement was carried out by applying a pressure of 2 Kgf/cm² onto aplanar indenter with a diameter of 1.8 mm at a heating rate of 5° C./minto prepare a TMA curve, from which a softening temperature (° C.) wasdetermined.

[Internal Haze (%)]

Using a press sheet with a thickness of 1 mm as a specimen, measurementwas carried out with a digital haze meter “NDH-20D”, manufactured byNippon Denshoku Industries, Ltd.

[MFR]

A MFR of the crystalline olefin resin (BB) was measured at 230° C. undera load of 2.16 kg in accordance with JIS K-6721.

A MFR of the α-olefin copolymer (CC) was measured in accordance with JISK-6721, at 190° C. under a load of 2.16 kg for an ethylene/α-olefincopolymer and a butene/α-olefin copolymer, and at 230° C. under a loadof 2.16 kg for a propylene/α-olefin copolymer.

[Density]

In accordance with ASTM D 1505 (water replacement method), using anelectronic densimeter manufactured by ALFA MIRAGE Co., Ltd., a densitywas calculated from a weight of a specimen measured in water and aweight of a specimen measured in air.

[Ball Drop Resilience Ratio]

A press sheet with a thickness of 6 mm was prepared. Then, under a roomtemperature of 25° C. or under 40° C., in accordance with JIS K6400, arigid ball of 16.310 g was dropped thereon from a height of 460 mm, anda rebound height at this time was measured. A ratio of the reboundheight to the height at which the ball was dropped was calculated as aball drop resilience ratio.

Example 1

Into a SUS autoclave with an agitating element having a volume of 1.5 Lthat had been sufficiently purged with nitrogen, at 23° C., 750 mL of4-methyl-1-pentene was introduced. Into this autoclave, 0.75 mL of atoluene solution of 1.0 mmol/mL of triisobutylaluminum (TIBAl) wasintroduced, and the agitator was operated. Then, the autoclave washeated till the temperature of the mixture became 30° C., andpressurization using propylene was performed such that the totalpressure became 0.74 MPaG. Then, 0.34 mL of a previously-preparedtoluene solution containing 1 mmol in terms of Al of methylaluminoxaneand 0.005 mmol of diphenylmethylene (1-ethyl-3-t-butyl-cyclopentadienyl)(2,7-di-t-butyl-fluorenyl)zirconiumdichloride was injected usingnitrogen into the autoclave, thereby initiating polymerization. For thefollowing 60 minutes, temperature of the autoclave was controlled suchthat the temperature of the mixture was 60° C. At 60 minutes past theinitiation of the polymerization, 5 mL of methanol was injected usingnitrogen into the autoclave, thereby terminating the polymerization anddepressurizing the autoclave to atmospheric pressure. Into the reactionsolution, acetone was poured with stirring. The resultantsolvent-containing rubber polymer was dried at 130° C. under reducedpressure for 12 hours.

The resultant polymer weighed 56.3 g, and the content of propylene inthe polymer was 75.3 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.5 dL/g; the molecular weightdistribution obtained by GPC was such that Mw was 287000, Mn was 144000,and Mw/Mn was 2.0; the extracted amount under methyl acetate was 0.6 wt%; YM was 1 MPa; ΔHS was 14; and the maximum value of tan δ was 3.5(temperature giving the maximum value: 6° C.). Properties of theresultant polymer are shown in Table 1.

Example 2

Into a SUS autoclave with an agitating element having a volume of 1.5 Lthat had been sufficiently purged with nitrogen, at 23° C., 750 mL of4-methyl-1-pentene (4MP1) was introduced. Into this autoclave, 0.75 mLof a toluene solution of 1.0 mmol/mL of triisobutylaluminum (TIBAl) wasintroduced, and the agitator was operated. Then, the autoclave washeated till the temperature of the mixture became 30° C., andpressurization using propylene was performed such that the totalpressure became 0.68 MPaG. Then, 0.34 mL of a previously-preparedtoluene solution containing 1 mmol in terms of Al of methylaluminoxaneand 0.005 mmol of diphenylmethylene(1-methyl-3-t-butyl-cyclopentadienyl)(2,7-di-t-butyl-fluorenyl)zirconiumdichloride was injected usingnitrogen into the autoclave, thereby initiating polymerization. For thefollowing 60 minutes, temperature of the autoclave was controlled suchthat the temperature of the mixture was 60° C. At 60 minutes past theinitiation of the polymerization, 5 mL of methanol was injected usingnitrogen into the autoclave, thereby terminating the polymerization anddepressurizing the autoclave to atmospheric pressure. Into the reactionsolution, acetone was poured with stirring. The resultantsolvent-containing rubber polymer was dried at 130° C. under reducedpressure for 12 hours.

The resultant polymer weighed 45.9 g, and the content of propylene inthe polymer was 68.9 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.47 dL/g; the molecularweight distribution obtained by GPC was such that Mw was 310000, Mn was155000, and Mw/Mn was 2.0; the extracted amount under methyl acetate was0.2 wt %; YM was 1 MPa; ΔHS was 24; and the maximum value of tan δ was3.2 (temperature giving the maximum value: 11° C.). Properties of theresultant polymer are shown in Table 1.

Example 3

Polymerization was performed in the same manner as in Example 2, exceptthat the pressurization using propylene was performed such that thetotal pressure in the polymerization container was 0.35 MPaG.

The resultant polymer weighed 46.9 g, and the content of propylene inthe polymer was 52.7 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.41 dL/g; the molecularweight distribution obtained by GPC was such that Mw was 285000, Mn was143000, and Mw/Mn was 2.0; the extracted amount under methyl acetate was0.2 wt %; YM was 3 MPa; ΔHS was 38; and the maximum value of tan δ was3.4 (temperature giving the maximum value: 19° C.). Properties of theresultant polymer are shown in Table 1.

Example 4

Polymerization was performed in the same manner as in Example 1, exceptthat the pressurization using propylene was performed such that thetotal pressure in the polymerization container was 0.20 MPaG.

The resultant polymer weighed 35.5 g, and the content of propylene inthe polymer was 40.0 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.4 dL/g; the molecular weightobtained by GPC was such that Mw was 272000, Mn was 131000, and Mw/Mnwas 2.1; the extracted amount under methyl acetate was 0.3 wt %; YM was15 MPa; ΔHS was 39; and the maximum value of tan δ was 3.0 (temperaturegiving the maximum value: 24° C.). Properties of the resultant polymerare shown in Table 1.

Example 5

Polymerization was performed in the same manner as in Example 2, exceptthat the pressurization using propylene was performed such that thetotal pressure in the polymerization container was 0.15 MPaG.

The resultant polymer weighed 46.9 g, and the content of propylene inthe polymer was 38.0 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.44 dL/g; the molecularweight distribution obtained by GPC was such that Mw was 295000, Mn was142000, and Mw/Mn was 2.09; the extracted amount under methyl acetatewas 0.2 wt %; YM was 80 MPa; ΔHS was 40; and the maximum value of tan δwas 2.8 (temperature giving the maximum value: 25° C.). Properties ofthe resultant polymer are shown in Table 1.

Example 6

Polymerization was performed in the same manner as in Example 2, exceptthat the pressurization using propylene was performed such that thetotal pressure in the polymerization container was 0.15 MPaG, and thepolymerization temperature was 60° C.

The resultant polymer weighed 24.0 g, and the content of propylene inthe polymer was 29.1 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.31 dL/g; the molecularweight obtained by GPC was such that Mw was 257000, Mn was 124000, andMw/Mn was 2.08; the extracted amount under methyl acetate was 0.2 wt %;YM was 176 MPa; ΔHS was 24; and the maximum value of tan δ was 2.5(temperature giving the maximum value: 26° C.). Properties of theresultant polymer are shown in Table 1.

Example 7

Polymerization was performed in the same manner as in Example 1, exceptthat the pressurization using propylene was performed such that thetotal pressure in the polymerization container was 0.13 MPaG, and thepolymerization temperature was 60° C.

The resultant polymer weighed 22.6 g, and the content of propylene inthe polymer was 28.1 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.39 dL/g; the molecularweight obtained by GPC was such that Mw was 290000, Mn was 138000, andMw/Mn was 2.10; the extracted amount under methyl acetate was 0.4 wt %;YM was 72 MPa; ΔHS was 31; and the maximum value of tan δ was 2.2(temperature giving the maximum value: 30° C.). Properties of theresultant polymer are shown in Table 1.

Example 8

Polymerization was performed in the same manner as in Example 4, exceptthat 100 mL of 4-methyl-1-pentene and 650 mL of n-hexane were introducedinto the polymerization container and then the pressurization usingpropylene was performed such that the total pressure in thepolymerization container was 0.68 MPaG, and the polymerizationtemperature was 60° C.

The resultant polymer weighed 35.3 g, and the content of propylene inthe polymer was 88.0 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.61 dL/g; the molecularweight obtained by GPC was such that Mw was 320000, Mn was 153000, andMw/Mn was 2.09; YM was 33 MPa; ΔHS was 29; and the maximum value of tanδ was 0.7 (temperature giving the maximum value: 6° C.). Properties ofthe resultant polymer are shown in Table 1.

Example 9

Polymerization was performed in the same manner as in Example 2, exceptthat diphenylmethylene (1-methyl-3-t-butyl-cyclopentadienyl)(2,7-di-t-butyl-fluorenyl)zirconiumdichloride was replaced withdi-p-chlorophenylene (cyclopentadienyl) (1,1,4,4,7,7,10,10-octamethyl-1,2,3,4,7,8,9,10-octahydrodibenz(b,h)-fluorenyl)zirconiumdichloride,and the polymerization temperature was 60° C.

The resultant polymer weighed 17.5 g, and the content of propylene inthe polymer was 67.2 mol %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.01 dL/g; the molecularweight distribution obtained by GPC was such that Mw was 210000, Mn was104000, and Mw/Mn was 2.02; YM was 1 MPa; ΔHS was 36; and the maximumvalue of tan δ was 2.6 (temperature giving the maximum value: 20° C.).Properties of the resultant polymer are shown in Table 1.

Example 10

Into a SUS autoclave with an agitating element having a volume of 1.5 Lthat had been sufficiently purged with nitrogen, at 23° C., 750 mL of4-methyl-1-pentene was introduced. Into this autoclave, 0.75 mL of atoluene solution of 1.0 mmol/mL of triisobutylaluminum (TIBAl) wasintroduced, and the agitator was operated. Then, the autoclave washeated till the temperature of the mixture became 60° C., andpressurization using ethylene was performed such that the total pressurebecame 0.15 MPaG. Then, 0.1 mL of a previously-prepared toluene solutioncontaining 1.5 mmol in terms of Al of methylaluminoxane and 0.005 mmolof di-p-chlorophenylene (cyclopentadienyl) (1,1,4,4,7,7,10,10-octamethyl-1,2,3,4,7,8,9,10-octahydrodibenz(b,h)-fluorenyl)zirconiumdichloridewas injected using nitrogen into the autoclave, thereby initiatingpolymerization. For the following 30 minutes, temperature of theautoclave was controlled such that the temperature of the mixture was60° C. At 30 minutes past the initiation of the polymerization, 5 mL ofmethanol was injected using nitrogen into the autoclave, therebyterminating the polymerization and depressurizing the autoclave toatmospheric pressure. Into the reaction solution, acetone was pouredwith stirring. The resultant solvent-containing rubber polymer was driedat 130° C. under reduced pressure for 12 hours.

The resultant polymer weighed 24.8 g, and the content of ethylene in thepolymer was 21.0 mol %. With regard to the polymer, Tm was not observed;the intrinsic viscosity [η] was 1.0 dL/g; the molecular weight obtainedby GPC was such that Mw was 205000, Mn was 103000, and Mw/Mn was 1.99;YM was 1 MPa; ΔHS was 20; and the maximum value of tan δ was 0.7(temperature giving the maximum value: 23° C.). Properties of theresultant polymer are shown in Table 1.

Example 11

Polymerization was performed in the same manner as in Example 10, exceptthat the pressurization using ethylene was performed such that the totalpressure in the polymerization container was 0.68 MPaG.

The resultant polymer weighed 24.8 g, and the content of ethylene in thepolymer was 35.0 mol %. With regard to the polymer, Tm was not observed;the intrinsic viscosity [η] was 1.7 dL/g; the molecular weight obtainedby GPC was such that Mw was 335000, Mn was 157000, and Mw/Mn was 2.13;YM was 0.3 MPa; ΔHS was 30; and the maximum value of tan δ was 2.7(temperature giving the maximum value: 2° C.). Properties of theresultant polymer are shown in Table 1.

Example 12

Into a SUS autoclave with an agitating element having a volume of 1.5 Lthat had been sufficiently purged with nitrogen, at 23° C., 750 mL of4-methyl-1-pentene was introduced. Into this autoclave, 0.75 mL of atoluene solution of 1.0 mmol/mL of triisobutylaluminum (TIBAl) wasintroduced, and the agitator was operated. Then, 180 g of butene-1 wasinjected. The autoclave was heated till the temperature of the mixturebecame 60° C. Then, 0.75 mL of a previously-prepared toluene solutioncontaining 1 mmol in terms of Al of methylaluminoxane and 0.01 mmol ofdiphenylmethylene(1-methyl-3-t-butyl-cyclopentadienyl(2,7-di-t-butyl-fluorenyl)zirconiumdichloridewas injected using nitrogen into the autoclave, thereby initiatingpolymerization. For the following 40 minutes, temperature of theautoclave was controlled such that the temperature of the mixture was60° C. At 40 minutes past the initiation of the polymerization, 5 mL ofmethanol was injected using nitrogen into the autoclave, therebyterminating the polymerization and depressurizing the autoclave toatmospheric pressure. Into the reaction solution, acetone was pouredwith stirring. The resultant solvent-containing rubber polymer was driedat 130° C. under reduced pressure for 12 hours.

The resultant polymer weighed 59.4 g, and the content of butene in thepolymer was 42.0 mol %. With regard to the polymer, Tm was not observed;the intrinsic viscosity [η] was 1.41 dL/g; the molecular weightdistribution obtained by GPC was such that Mw was 290000, Mn was 145000,and Mw/Mn was 2.0; YM was 140 MPa; ΔHS was 16; and the maximum value oftan δ was 0.6 (temperature giving the maximum value: 5° C.). Propertiesof the resultant polymer are shown in Table 1.

Example 13

Into a SUS autoclave with an agitating element having a volume of 1.5 Lthat had been sufficiently purged with nitrogen, at 23° C., 750 mL of4-methyl-1-pentene and 4.5 mL of 5-ethylidene-2-norbornene (ENB) wereintroduced. Into this autoclave, 0.75 mL of a toluene solution of 1.0mmol/mL of triisobutylaluminum (TIBAl) was introduced, and the agitatorwas operated. Then, the autoclave was heated till the temperature of themixture became 60° C., and pressurization using ethylene was performedsuch that the total pressure became 0.63 MPaG. Then, 0.34 mL of apreviously-prepared toluene solution containing 0.020 mmol of (C₆H₅)₃CB(C₆F₅)₄ and 0.005 mmol of di-p-chlorophenylene (cyclopentadienyl)(1,1,4,4,7,7,10,10-octamethyl-1,2,3,4,7,8,9,10-octahydrodibenz(b,h)-fluorenyl)zirconiumdichloridewas injected using nitrogen into the autoclave, thereby initiatingpolymerization. For the following 30 minutes, temperature of theautoclave was controlled such that the temperature of the mixture was60° C. At 30 minutes past the initiation of the polymerization, 5 mL ofmethanol was injected using nitrogen into the autoclave, therebyterminating the polymerization and depressurizing the autoclave toatmospheric pressure. Into the reaction solution, acetone was pouredwith stirring. The resultant solvent-containing rubber polymer was driedat 80° C. under reduced pressure for 12 hours.

The resultant polymer weighed 26.0 g, and the content of ethylene in thepolymer was 53.4 mol %, and the content of ENB in the polymer was 1.6mol %. With regard to the polymer, Tm was not observed; the intrinsicviscosity [η] was 1.29 dL/g; the molecular weight distribution obtainedby GPC was such that Mw was 270000, Mn was 123000, and Mw/Mn was 2.2; YMwas 1 MPa; ΔHS was 22; and the maximum value of tan δ was 2.8(temperature giving the maximum value: −16° C.). Properties of theresultant polymer are shown in Table 1.

Comparative Example 1

Into a SUS autoclave with an agitating element having a volume of 1.5 Lthat had been sufficiently purged with nitrogen, at 23° C., 750 mL of4-methyl-1-pentene was introduced. Into this autoclave, 0.94 mL of atoluene solution of 1.0 mmol/mL of triethylaluminum (TEA) was introducedand 240 NmL of a hydrogen gas was introduced, and the agitator wasoperated. Then, the autoclave was heated till the temperature of themixture became 60° C., and pressurization using propylene was performedsuch that the total pressure became 0.43 MPaG. Then, 4.7 mL of a toluenesolution containing 0.013 mmol of a solid titanium catalyst prepared inaccordance with JP-A-2008-144155 was injected using nitrogen into theautoclave, thereby initiating polymerization. For the following 60minutes, temperature of the autoclave was controlled such that thetemperature of the mixture was 60° C. At 60 minutes past the initiationof the polymerization, 5 mL of methanol was injected using nitrogen intothe autoclave, thereby terminating the polymerization and depressurizingthe autoclave to atmospheric pressure. Into the reaction solution,acetone was poured with stirring. The resultant solvent-containingrubber polymer was dried at 130° C. under reduced pressure for 12 hours.

The resultant polymer weighed 77.1 g, and the content of propylene inthe polymer was 85.0 mol %. With regard to the polymer, Tm was 146.1°C.; the intrinsic viscosity [η] was 1.16 dL/g; Mw/Mn was 6.7; YM was 153MPa; ΔHS was 7; and the maximum value of tan δ was 0.5 (temperaturegiving the maximum value: 8° C.). Properties of the resultant polymerare shown in Table 1.

It is clear from the change in Shore A hardness and the peak value oftan δ that the stress absorption is inferior.

Comparative Example 2

By reference to Example 5 described in JP-A-2008-144155, a4-methyl-1-pentene/1-hexene copolymer was obtained.

The content of hexene in the polymer was 45.6 mol %. With regard to thepolymer, Tm was 165° C.; the intrinsic viscosity [η] was 2.3 dL/g; theextracted amount under methyl acetate was 1.5 wt %; YM was 153 MPa; ΔHSwas 11; and the maximum value of tan δ was 0.3 (temperature giving themaximum value: 1° C.). Properties of the resultant polymer are shown inTable 1.

It is clear from the extracted amount under methyl acetate that themoldability is inferior, and it is clear from the peak value of tan δthat the stress absorption is inferior.

Comparative Example 3

A commercially-available poly(4-methyl-1-pentene) (TPX RT-18,manufactured by Mitsui Chemicals, Inc.) was used. Properties are shownin Table 1. It is clear from the mechanical properties that theflexibility is inferior.

Comparative Example 4

A commercially-available poly(4-methyl-1-pentene) (TPX MX-002,manufactured by Mitsui Chemicals, Inc.) was used. Properties are shownin Table 1. It is clear from the peak value of tan δ that the stressabsorption is inferior.

Comparative Example 5

A commercially-available ethylene/propylene/α-olefin (an α-olefin otherthan 4MP1) copolymer (TAFMER A4085, manufactured by Mitsui Chemicals,Inc.) was used. Properties are shown in Table 1. It is clear from themechanical properties that the flexibility is inferior, and it is clearfrom the peak value of tan δ that the stress absorption is inferior.

Comparative Example 6

A commercially-available hydrogenated styrene/butadiene/styrenecopolymer (TAFTEC H1041, manufactured by Asahi Kasei Corporation) wasused. Properties are shown in Table 1.

It is clear from the change in Shore A hardness and the peak value oftan δ that the stress absorption is inferior.

TABLE 1 Ex. 1 Ex. 2 Ex. 3 Ex. 4 Ex. 5 Ex. 6 Ex. 7 Composition 4MP1 mol %25 31 47 60 62 71 72 α-olefin content (1) mol % 75 69 53 40 38 29 28α-olefin type propylene propylene propylene propylene propylenepropylene propylene α-olefin content (2) mol % α-olefin type B value 0.90.9 0.9 1.0 1.0 1.0 1.0 Molecular [η] dL/g 1.5 1.5 1.4 1.4 1.4 1.3 1.4weight Mw/Mn 2.0 2.0 2.0 2.1 2.1 2.1 2.1 Mw 287000 310000 285000 272000295000 257000 290000 Extracted amount % 0.6 0.2 0.2 0.3 0.2 0.2 0.4under methyl acetate Lightness Density kg/m³ 847 847 845 840 842 839 839Mechanical YM MPa 1 1 3 15 80 176 72 properties TS MPa 1 2 6 25 24 28 28EL % 1237 1116 672 646 573 523 537 Rubber elasticity PS % 24 13 6 3 6 915 Heat Tm ° C. Not Not Not Not Not Not Not resistance observed observedobserved observed observed observed observed Flexibility Shore hardness(immediately after) 40 52 72 88 94 96 95 Shore hardness (15 sec after)26 28 34 49 54 72 64 Hardness meter type A A A A A A A ΔHS 14 24 38 3940 24 31 Stress Temperature giving tan δ peak ° C. 6 11 19 24 25 26 30Absorption tan δ peak value 3.5 3.2 3.4 3.0 2.8 2.5 2.2 Ball dropresilience ratio (25° C.) % 1 2 22 27 38 40 30 (40° C.) % 12 2 1 1 4 4 2Abrasion Percentage of change in gloss 54 14 1 1 4 4 4 resistance ΔG (%)Ex. 8 Ex. 9 Ex. 10 Ex. 11 Ex. 12 Ex. 13 Com. Ex. 1 Composition 4MP1 mol% 12 33 79 65 58 45 15 α-olefin content (1) mol % 88 67 21 35 42 53 85α-olefin type propylene propylene ethylene ethylene butene ethylenepropylene α-olefin content (2) mol % 1.6 α-olefin type ENB B value 1.00.9 1.3 1.2 0.9 1.0 0.8 Molecular [η] dL/g 1.6 1.0 1.0 1.7 1.4 1.3 1.2weight Mw/Mn 2.1 2.0 2.0 2.1 2.0 2.2 6.7 Mw 320000 210000 205000 335000290000 270000 275000 Extracted amount % 0.4 0.3 0.2 0.4 0.3 0.4 1.8under methyl acetate Lightness Density kg/m³ 850 840 848 845 847 843 860Mechanical YM MPa 33 1 1 0.3 140 1 153 properties TS MPa 36 3 5 25 5 3 4EL % 763 1052 1307 925 310 712 213 Rubber elasticity PS % 6 11 3 76 HeatTm ° C. Not Not Not Not Not Not 146 resistance observed observedobserved observed observed observed Flexibility Shore hardness(immediately after) 92 94 95 90 96 62 89 Shore hardness (15 sec after)63 58 75 60 80 40 82 Hardness meter type A A A A A A A ΔHS 29 36 20 3016 22 7 Stress Temperature giving tan δ peak ° C. 6 20 23 2 5 −16 8Absorption tan δ peak value 0.7 2.6 0.7 2.7 0.6 2.8 0.5 Ball dropresilience ratio (25° C.) % 7 38 25 2 17 2 20 (40° C.) % 21 5 5 8 22 1626 Abrasion Percentage of change in gloss 18 2 4 1 resistance ΔG (%)Com. Ex. 1 Com. Ex. 2 Com. Ex. 3 Com. Ex. 4 Com. Ex. 5 Com. Ex. 6Composition 4MP1 mol % 15 α-olefin content(1) mol % 85 α-olefin typepropylene α-olefin content (2) mol % α-olefin type B value 0.8 Molecular[η] dL/g 1.2 weight Mw/Mn 6.7 Mw 275000 Extracted amount under methyl %1.8 1.5 acetate Lightness Density kg/m³ 860 840 A833 835 885 910Mechanical YM MPa 153 153 1324 691 4 57 properties TS MPa 4 5 24 22 2722 EL % 213 209 24 338 800 650 Rubber elasticity PS % 76 Heat resistanceTm ° C. 146 165 237 222 73 105 Flexibility Shore hardness (immediatelyafter) 89 95 75 64 83 84 Shore hardness (15 sec after) 82 84 74 62 82 80Hardness meter type A A D D A A ΔHS 7 11 1 2 1 4 Stress Temperaturegiving tan δ peak ° C. 8 1 32 31 −27 −43 Absorption tan δ peak value 0.50.3 0.3 0.2 0.3 0.3 Ball drop resilience ratio (25° C.) % 20 25 35 28 4140 (40° C.) % 26 28 24 22 48 45 Abrasion Percentage of change in gloss 23 2 94 30 resistance ΔG (%)

Example 14

83 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 2 was blended with 17 parts by weight of Clearon P-125, aterpene-based hydrogenated resin manufactured by Yasuhara Chemical Co.,Ltd. Further, 100 parts by weight of the composition was blended with1000 ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000 ppmof Irgafos 168, a phosphorus-based processing heat stabilizer, each ofwhich is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 2.

It is clear from the large change ΔHS in Shore A hardness that thestress absorption is excellent, and it is clear from the peak value oftan δ (tan δ: 2.8, temperature giving the maximum value: 20° C.) thatthe stress absorption is excellent.

Example 15

83 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 17 parts by weight of Clearon P-125, aterpene-based hydrogenated resin manufactured by Yasuhara Chemical Co.,Ltd. Further, 100 parts by weight of the composition was blended with1000 ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000 ppmof Irgafos 168, a phosphorus-based processing heat stabilizer, each ofwhich is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 2.

It is clear from the large change ΔHS(=20) in Shore A hardness that thestress absorption is excellent, and it is clear from the peak value oftan δ (tan δ: 2.6, temperature giving the maximum value: 28° C.) thatthe stress absorption is excellent.

Example 16

60 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 40 parts by weight of TAFTEC H1041, ahydrogenated styrene-based thermoplastic elastomer manufactured by AsahiKasei Corporation. Further, 100 parts by weight of the composition wasblended with 1000 ppm of Irganox 1010, a hindered phenol-basedantioxidant, 1000 ppm of Irgafos 168, a phosphorus-based processing heatstabilizer, each of which is manufactured by Ciba Japan K.K., and 500ppm of calcium stearate manufactured by NOF Corporation. Then, thesewere melt kneaded using a Labo Plastomill (a biaxial batch type meltkneading apparatus) manufactured by Toyo Seiki Seisaku-Sho Ltd., withthe temperature set at 200° C., with the resins charged in an amount of40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5 minutes. Then,the mixture was collected and cooled using a cooling press set at 20°C., to thereby form a sheet. The sheet was cut so as to have anappropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 2.

It is clear from the large change ΔHS(=22) in Shore A hardness that thestress absorption is excellent, and it is clear from the peak value oftan δ (tan δ: 0.8, temperature giving the maximum value: 22° C.) thatthe stress absorption is excellent.

Example 17

80 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 20 parts by weight of PW-100, a processoil manufactured by Idemitsu Kosan Co., Ltd. Further, 100 parts byweight of the composition was blended with 1000 ppm of Irganox 1010, ahindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 2.

It is clear from the large change ΔHS in Shore A hardness that thestress absorption is excellent, and it is clear from the peak value oftan δ (tan δ: 3.3, temperature giving the maximum value: 7° C.) that thestress absorption is excellent.

Example 18

60 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 40 parts by weight of PW-100, a processoil manufactured by Idemitsu Kosan Co., Ltd. Further, 100 parts byweight of the composition was blended with 1000 ppm of Irganox 1010, ahindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 2.

It is clear from the large change ΔHS in Shore A hardness that thestress absorption is excellent, and it is clear from the peak value oftan δ (tan δ: 2.8, temperature giving the maximum value: −11° C.) thatthe stress absorption is excellent.

TABLE 2 Ex. 14 Ex. 15 Ex. 16 Ex. 17 Ex. 18 Polymer (A) Ex. 2 Ex. 5 Ex. 5Ex. 5 Ex. 5 Thermoplastic resin (B) P-125 P-125 H1041 PW-100 PW-100 (A)/ (B) compositional 83/17 83/17 60/40 80/20 60/40 ratio (wt %) YM 2 8670 1 0.1 TS 5 20 20 0.3 0.1 EL 869 495 450 1031 1200 Shore hardness 7195 94 32 15 (immediately after) Shore hardness 29 75 72 16 4 (15 secafter) Hardness meter A A A A A ΔHS 42 20 22 7 −11 Temperature giving 2028 22 7 −11 tan δ peak (° C.) tan δ peak value 2.8 2.6 0.8 3.3 2.8 Balldrop resilience 7 38 36 3 21 ratio (25° C.) (%) Ball drop resilience 101 4 2 3 ratio (40° C.) (%) Internal Haze 2 12 33 10 11

Example 19

20 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 2 was blended with 80 parts by weight of F107P, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, 100 partsby weight of the composition was blended with 1000 ppm of Irganox 1010,a hindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 3.

It is clear from the large elongation that the modification property isexcellent, and it is clear from the percentage of change in gloss thatthe abrasion resistance is excellent, and further it is clear from thesoftening temperature that the heat resistance is excellent. It is alsoclear that the transparency is not impaired.

Example 20

40 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 2 was blended with 60 parts by weight of F107P, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, 100 partsby weight of the composition was blended with 1000 ppm of Irganox 1010,a hindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 3.

It is clear from the large elongation that the modification property isexcellent, and it is clear from the percentage of change in gloss thatthe abrasion resistance is excellent, and further it is clear from thesoftening temperature that the heat resistance is excellent.

Example 21

20 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 80 parts by weight of F107P, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, 100 partsby weight of the composition was blended with 1000 ppm of Irganox 1010,a hindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 3.

It is clear from the large elongation that the modification property isexcellent, and it is clear from the percentage of change in gloss thatthe abrasion resistance is excellent, and further it is clear from thesoftening temperature that the heat resistance is excellent.

Example 22

20 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 2 was blended with 80 parts by weight ofpoly(4-methyl-1-pentene) (TPX RT-18, manufactured by Mitsui Chemicals,Inc., a homopolymer). Further, 100 parts by weight of the compositionwas blended with 1000 ppm of Irganox 1010, a hindered phenol-basedantioxidant, 1000 ppm of Irgafos 168, a phosphorus-based processing heatstabilizer, each of which is manufactured by Ciba Japan K.K., and 500ppm of calcium stearate manufactured by NOF Corporation. Then, thesewere melt kneaded using a Labo Plastomill (a biaxial batch type meltkneading apparatus) manufactured by Toyo Seiki Seisaku-Sho Ltd., withthe temperature set at 260° C., with the resins charged in an amount of40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5 minutes. Then,the mixture was collected and cooled using a cooling press set at 20°C., to thereby form a sheet. The sheet was cut so as to have anappropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 3.

It is clear from the large elongation that the modification property isexcellent, and it is clear from the percentage of change in gloss thatthe abrasion resistance is excellent, and further it is clear from thesoftening temperature that the heat resistance is excellent.

Example 23

20 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 80 parts by weight ofpoly(4-methyl-1-pentene) (TPX RT-18, manufactured by Mitsui ChemicalsInc.). Further, 100 parts by weight of the composition was blended with1000 ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000 ppmof Irgafos 168, a phosphorus-based processing heat stabilizer, each ofwhich is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at260° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 3.

It is clear from the large elongation that the modification property isexcellent, and it is clear from the percentage of change in gloss thatthe abrasion resistance is excellent, and further it is clear from thesoftening temperature that the heat resistance is excellent. It is alsoclear that the transparency is not impaired.

Example 24

40 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 60 parts by weight ofpoly(4-methyl-1-pentene) (TPX RT-18, manufactured by Mitsui ChemicalsInc.). Further, 100 parts by weight of the composition was blended with1000 ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000 ppmof Irgafos 168, a phosphorus-based processing heat stabilizer, each ofwhich is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at260° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 3.

It is clear from the large elongation that the modification property isexcellent, and it is clear from the percentage of change in gloss thatthe abrasion resistance is excellent, and further it is clear from thesoftening temperature that the heat resistance is excellent. It is alsoclear that the transparency is not impaired.

Comparative Example 7

20 parts by weight of the ethylene/α-olefin copolymer shown inComparative Example 5 was blended with 80 parts by weight of F107P, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, 100 partsby weight of the composition was blended with 1000 ppm of Irganox 1010,a hindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 3.

It is clear that the percentage of change in gloss is higher as comparedwith Examples, and the transparency is impaired.

Comparative Example 8

20 parts by weight of the ethylene/α-olefin copolymer shown inComparative Example 5 was blended with 80 parts by weight ofpoly(4-methyl-1-pentene) (TPX RT-18, manufactured by Mitsui ChemicalsInc.). Further, 100 parts by weight of the composition was blended with1000 ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000 ppmof Irgafos 168, a phosphorus-based processing heat stabilizer, each ofwhich is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at260° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 3.

It is clear that the percentage of change in gloss is higher, thetransparency is lower, and the elongation is inferior, as compared withExamples.

TABLE 3 Ex. 19 Ex. 20 Ex. 21 Ex. 22 Ex. 23 Ex. 24 Com. Ex. 7 Com. Ex. 8Polymer (A) Ex. 2 Ex. 2 Ex. 5 Ex. 2 Ex. 5 Ex. 5 Com. Ex. 5 Com. Ex. 5Thermoplastic resin (B) F107P F107P F107P RT-18 RT-18 RT-18 F107 RT-18(A)/(B) compositional ratio (wt %) 20/80 40/60 20/80 20/80 20/80 40/6020/80 20/80 Percentage of change in gloss ΔG % 3 1 1 10 3 0 30 30 Tm °C. 162 162 162 236 236 236 162 236 Softening temperature ° C. 158 156160 235 231 228 160 235 YS MPa 25 14 26 19 19 13 27 25 EL % 668 750 621154 295 257 1000 56 TS MPa 39 35 42 17 26 21 40 21 YM MPa 960 660 11291086 964 610 1080 1100 Internal Haze % 57 70 93 34 13 16 93 91

Example 25

90 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 1 was blended with 10 parts by weight of F107P, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, 100 partsby weight of the composition was blended with 1000 ppm of Irganox 1010,a hindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=13) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.7, temperature giving the maximumvalue: 6.4° C.) that the stress absorption is excellent.

Example 26

70 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 1 was blended with 30 parts by weight of F107P, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, 100 partsby weight of the composition was blended with 1000 ppm of Irganox 1010,a hindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=8) in Shore A hardness and thehigh peak value of tan δ (tan δ: 0.9, temperature giving the maximumvalue: 6.6° C.) that the stress absorption is excellent.

Example 27

80 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 1 was blended with 20 parts by weight of PRIME TPOM2606,manufactured by Prime Polymer Co., Ltd. Further, 100 parts by weight ofthe composition was blended with 1000 ppm of Irganox 1010, a hinderedphenol-based antioxidant, 1000 ppm of Irgafos 168, a phosphorus-basedprocessing heat stabilizer, each of which is manufactured by Ciba JapanK.K., and 500 ppm of calcium stearate manufactured by NOF Corporation.Then, these were melt kneaded using a Labo Plastomill (a biaxial batchtype melt kneading apparatus) manufactured by Toyo Seiki Seisaku-ShoLtd., with the temperature set at 200° C., with the resins charged in anamount of 40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5minutes. Then, the mixture was collected and cooled using a coolingpress set at 20° C., to thereby form a sheet. The sheet was cut so as tohave an appropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 4.

It is clear from the large change (ΔHS=15) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.7, temperature giving the maximumvalue: 6.3° C.) that the stress absorption is excellent.

Example 28

60 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 1 was blended with 40 parts by weight of PRIME TPOM2606,manufactured by Prime Polymer Co., Ltd. Further, 100 parts by weight ofthe composition was blended with 1000 ppm of Irganox 1010, a hinderedphenol-based antioxidant, 1000 ppm of Irgafos 168, a phosphorus-basedprocessing heat stabilizer, each of which is manufactured by Ciba JapanK.K., and 500 ppm of calcium stearate manufactured by NOF Corporation.Then, these were melt kneaded using a Labo Plastomill (a biaxial batchtype melt kneading apparatus) manufactured by Toyo Seiki Seisaku-ShoLtd., with the temperature set at 200° C., with the resins charged in anamount of 40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5minutes. Then, the mixture was collected and cooled using a coolingpress set at 20° C., to thereby form a sheet. The sheet was cut so as tohave an appropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 4.

It is clear from the large change (ΔHS=10) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.0, temperature giving the maximumvalue: 8.8° C.) that the stress absorption is excellent.

Example 29

70 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 1 was blended with 30 parts by weight of TAFMER XM7070,manufactured by Mitsui Chemicals, Inc. Further, 100 parts by weight ofthe composition was blended with 1000 ppm of Irganox 1010, a hinderedphenol-based antioxidant, 1000 ppm of Irgafos 168, a phosphorus-basedprocessing heat stabilizer, each of which is manufactured by Ciba JapanK.K., and 500 ppm of calcium stearate manufactured by NOF Corporation.Then, these were melt kneaded using a Labo Plastomill (a biaxial batchtype melt kneading apparatus) manufactured by Toyo Seiki Seisaku-ShoLtd., with the temperature set at 200° C., with the resins charged in anamount of 40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5minutes. Then, the mixture was collected and cooled using a coolingpress set at 20° C., to thereby form a sheet. The sheet was cut so as tohave an appropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 4.

It is clear from the large change (ΔHS=15) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.1, temperature giving the maximumvalue: 6.4° C.) that the stress absorption is excellent.

Example 30

80 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 2 was blended with 20 parts by weight of F107P, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, 100 partsby weight of the composition was blended with 1000 ppm of Irganox 1010,a hindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=17) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.1, temperature giving the maximumvalue: 10° C.) that the stress absorption is excellent.

Example 31

80 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 3 was blended with 20 parts by weight ofpoly(4-methyl-1-pentene) (TPX RT-18, manufactured by Mitsui ChemicalsInc.). Further, 100 parts by weight of the composition was blended with1000 ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000 ppmof Irgafos 168, a phosphorus-based processing heat stabilizer, each ofwhich is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at260° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=21) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.7, temperature giving the maximumvalue: 12° C.) that the stress absorption is excellent.

Example 32

80 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 20 parts by weight of F107P, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, 100 partsby weight of the composition was blended with 1000 ppm of Irganox 1010,a hindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=24) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.9, temperature giving the maximumvalue: 25° C.) that the stress absorption is excellent.

Example 33

80 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 5 was blended with 20 parts by weight ofpoly(4-methyl-1-pentene) (TPX RT-18, manufactured by Mitsui ChemicalsInc.). Further, 100 parts by weight of the composition was blended with1000 ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000 ppmof Irgafos 168, a phosphorus-based processing heat stabilizer, each ofwhich is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at260° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=20) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.5, temperature giving the maximumvalue: 25° C.) that the stress absorption is excellent.

Example 34

65 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 1 was blended with 35 parts by weight of HYBRAR 5127, ahydrogenated styrene/isoprene/styrene copolymer manufactured by KurarayCo., Ltd. Further, the resultant mixture was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=20) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.2, temperature giving the maximumvalue: 16° C.) that the stress absorption is excellent.

Example 35

20 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 1 was blended with 80 parts by weight of HYBRAR 5127, ahydrogenated styrene/isoprene/styrene copolymer manufactured by KurarayCo., Ltd. Further, the resultant mixture was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=22) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.3, temperature giving the maximumvalue: 19° C.) that the stress absorption is excellent.

Example 36

65 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 4 was blended with 35 parts by weight of HYBRAR 5127, ahydrogenated styrene/isoprene/styrene copolymer manufactured by KurarayCo., Ltd. Further, the resultant mixture was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=39) in Shore A hardness and thehigh peak value of tan δ (tan δ: 2.2, temperature giving the maximumvalue: 24° C.) that the stress absorption is excellent.

Example 37

20 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 4 was blended with 80 parts by weight of HYBRAR 5127, ahydrogenated styrene/isoprene/styrene copolymer manufactured by KurarayCo., Ltd. Further, the resultant mixture was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=26) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.2, temperature giving the maximumvalue: 21° C.) that the stress absorption is excellent.

Example 38

80 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 4 was blended with 20 parts by weight of a poly-1-butenemanufactured by Mitsui Chemicals, Inc. (TAFMER BL P5000). Further, theresultant mixture was blended with 1000 ppm of Irganox 1010, a hinderedphenol-based antioxidant, 1000 ppm of Irgafos 168, a phosphorus-basedprocessing heat stabilizer, each of which is manufactured by Ciba JapanK.K., and 500 ppm of calcium stearate manufactured by NOF Corporation.Then, these were melt kneaded using a Labo Plastomill (a biaxial batchtype melt kneading apparatus) manufactured by Toyo Seiki Seisaku-ShoLtd., with the temperature set at 200° C., with the resins charged in anamount of 40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5minutes. Then, the mixture was collected and cooled using a coolingpress set at 20° C., to thereby form a sheet. The sheet was cut so as tohave an appropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 4.

It is clear from the large change (ΔHS=26) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.4, temperature giving the maximumvalue: 19° C.) that the stress absorption is excellent.

Example 39

90 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 4 was blended with 10 parts by weight of a poly-1-butenemanufactured by Mitsui Chemicals, Inc. (TAFMER BL P5000). Further, theresultant mixture was blended with 1000 ppm of Irganox 1010, a hinderedphenol-based antioxidant, 1000 ppm of Irgafos 168, a phosphorus-basedprocessing heat stabilizer, each of which is manufactured by Ciba JapanK.K., and 500 ppm of calcium stearate manufactured by NOF Corporation.Then, these were melt kneaded using a Labo Plastomill (a biaxial batchtype melt kneading apparatus) manufactured by Toyo Seiki Seisaku-ShoLtd., with the temperature set at 200° C., with the resins charged in anamount of 40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5minutes. Then, the mixture was collected and cooled using a coolingpress set at 20° C., to thereby form a sheet. The sheet was cut so as tohave an appropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 4.

It is clear from the large change (ΔHS=35) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.9, temperature giving the maximumvalue: 20° C.) that the stress absorption is excellent.

Example 40

90 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 3 was blended with 10 parts by weight of a poly-1-butenemanufactured by Mitsui Chemicals, Inc. (TAFMER BL P5000). Further, theresultant mixture was blended with 1000 ppm of Irganox 1010, a hinderedphenol-based antioxidant, 1000 ppm of Irgafos 168, a phosphorus-basedprocessing heat stabilizer, each of which is manufactured by Ciba JapanK.K., and 500 ppm of calcium stearate manufactured by NOF Corporation.Then, these were melt kneaded using a Labo Plastomill (a biaxial batchtype melt kneading apparatus) manufactured by Toyo Seiki Seisaku-ShoLtd., with the temperature set at 200° C., with the resins charged in anamount of 40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5minutes. Then, the mixture was collected and cooled using a coolingpress set at 20° C., to thereby form a sheet. The sheet was cut so as tohave an appropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 4.

It is clear from the large change (ΔHS=32) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.8, temperature giving the maximumvalue: 19° C.) that the stress absorption is excellent.

Example 41

90 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 4 was blended with 10 parts by weight of E-200GP, apolypropylene manufactured by Prime Polymer Co., Ltd. Further, theresultant mixture was blended with 1000 ppm of Irganox 1010, a hinderedphenol-based antioxidant, 1000 ppm of Irgafos 168, a phosphorus-basedprocessing heat stabilizer, each of which is manufactured by Ciba JapanK.K., and 500 ppm of calcium stearate manufactured by NOF Corporation.Then, these were melt kneaded using a Labo Plastomill (a biaxial batchtype melt kneading apparatus) manufactured by Toyo Seiki Seisaku-ShoLtd., with the temperature set at 200° C., with the resins charged in anamount of 40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5minutes. Then, the mixture was collected and cooled using a coolingpress set at 20° C., to thereby form a sheet. The sheet was cut so as tohave an appropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 4.

It is clear from the large change (ΔHS=37) in Shore A hardness and thehigh peak value of tan δ (tan δ: 2.5, temperature giving the maximumvalue: 22° C.) that the stress absorption is excellent.

Example 42

90 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 4 was blended with 10 parts by weight of BL2481, apoly-1-butene copolymer manufactured by Mitsui Chemicals, Inc. Further,the resultant mixture was blended with 1000 ppm of Irganox 1010, ahindered phenol-based antioxidant, 1000 ppm of Irgafos 168, aphosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 4.

It is clear from the large change (ΔHS=33) in Shore A hardness and thehigh peak value of tan δ (tan δ: 1.4, temperature giving the maximumvalue: 20° C.) that the stress absorption is excellent.

Example 43

90 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 4 was blended with 10 parts by weight of TAFMER XM7070manufactured by Mitsui Chemicals, Inc. Further, the resultant mixturewas blended with 1000 ppm of Irganox 1010, a hindered phenol-basedantioxidant, 1000 ppm of Irgafos 168, a phosphorus-based processing heatstabilizer, each of which is manufactured by Ciba Japan K.K., and 500ppm of calcium stearate manufactured by NOF Corporation. Then, thesewere melt kneaded using a Labo Plastomill (a biaxial batch type meltkneading apparatus) manufactured by Toyo Seiki Seisaku-Sho Ltd., withthe temperature set at 200° C., with the resins charged in an amount of40 g (apparatus batch volume=60 cm³), at 50 rpm, for 5 minutes. Then,the mixture was collected and cooled using a cooling press set at 20°C., to thereby form a sheet. The sheet was cut so as to have anappropriate size, thereby preparing a specimen for measurement.Furthermore, using the specimen, a press sheet was prepared andproperties were measured. Results of various measurements are shown inTable 4.

It is clear from the large change (ΔHS=33) in Shore A hardness and thehigh peak value of tan δ (tan δ: 2.4, temperature giving the maximumvalue: 21° C.) that the stress absorption is excellent.

Comparative Example 2

Comparative Example 2 is also shown in Table 4 for reference.

TABLE 4 Ex. 25 Ex. 26 Ex. 27 Ex. 28 Ex. 29 Ex. 30 Ex. 31 Polymer (A) Ex.1 Ex. 1 Ex. 1 Ex. 1 Ex. 1 Ex. 2 Ex. 3 Thermoplastic resin (B) F107PF107P M2606 M2606 XM-7070 F107P RT-18 (A)/(B) compositional ratio (wt %)90/10 70/30 80/20 60/40 70/30 80/20 80/20 EL % 853 548 819 862 888 903757 TS MPa 9 16 5 16 32 20 5 YM MPa 4 30 3 12 71 4 5 Melting point (Tm)° C. 162 162 160 160 70 162 236 Shore hardness (immediately after) 58 8656 76 76 79 73 Shore hardness (15 sec after) 45 78 41 64 61 62 52Hardness meter type A A A A A A A ΔHS 13 8 15 10 15 17 21 Temperaturegiving tan δ peak ° C. 6.4 6.6 6.3 8.8 6.4 10 12 tan δ peak value 1.70.9 1.7 1.0 1.1 1.1 1.7 Ball drop resilience ratio (25° C.) % 3 8 4 7 65 2 Ball drop resilience ratio (40° C.) % 14 18 14 20 12 26 21 Ex. 32Ex. 33 Ex. 34 Ex. 35 Ex. 36 Ex. 37 Polymer (A) Ex. 5 Ex. 5 Ex. 1 Ex. 1Ex. 4 Ex. 4 Thermoplastic resin (B) F107P RT-18 HYBRAR HYBRAR HYBRARHYBRAR 5127 5127 5127 5127 (A)/(B) compositional ratio (wt %) 80/2080/20 65/35 20/80 65/35 20/80 EL % 571 519 707 672 656 687 TS MPa 30 265 12 25 21 YM MPa 128 125 2 8 15 20 Melting point (Tm) ° C. 162 236 100100 100 100 Shore hardness (immediately after) 89 90 56 81 83 85 Shorehardness (15 sec after) 65 70 36 59 44 59 Hardness meter type A A A A AA ΔHS 24 20 20 22 39 26 Temperature giving tan δ peak ° C. 25 25 16 1924 21 tan δ peak value 1.9 1.5 1.2 1.3 2.2 1.2 Ball drop resilienceratio (25° C.) % 31 33 4 8 14 10 Ball drop resilience ratio (40° C.) % 76 16 20 33 27 Ex. 38 Ex. 39 Ex. 40 Ex. 41 Ex. 42 Ex. 43 Com. Ex. 2Polymer (A) Ex. 4 Ex. 4 Ex. 3 Ex. 4 Ex. 4 Ex. 4 Com. Ex. 2 Thermoplasticresin (B) P5000 P5000 P5000 E-200GP BL2481 XM-7070 (A)/(B) compositionalratio (wt %) 80/20 90/10 90/10 90/10 90/10 90/10 100 EL % 725 656 658721 744 670 209 TS MPa 21 12 12 16 16 11 5 YM MPa 9 4 4 2 7 2 153Melting point (Tm) ° C. 120 120 120 160 75 70 165 Shore hardness(immediately after) 80 76 75 77 80 69 95 Shore hardness (15 sec after)54 41 43 40 47 36 84 Hardness meter A A A A A A A ΔHS 26 35 32 37 33 3311 Temperature giving tan δ peak ° C. 19 20 19 22 20 21 1 tan δ peakvalue 1.4 1.9 1.8 2.5 1.4 2.4 0.3 Ball drop resilience ratio (25° C.)(%) % 25 Ball drop resilience ratio (40° C.) (%) % 28

Example 44

15 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer obtainedin Example 1 and 140 parts by weight of anethylene/propylene/5-ethylidene-2-norbornene ternary copolymer [productname: Mitsui EPT3072EM, manufactured by Mitsui Chemicals, Inc.] werekneaded with 5 parts by weight of zinc oxide No. 2 (product name; zincoxide No. 2, manufactured by Hakusuitech Ltd.) as a vulcanizationpromoting assistant, 1 part by weight of stearic acid as a processingassistant, 47 parts by weight of “Diana Process Oil PW-380” (productname; manufactured by Idemitsu Kosan, Co., Ltd.) as a softener, and 80parts by weight of carbon black (product name: SEAST G116, manufacturedby Tokai Carbon Co., Ltd.). Kneading conditions were such that thenumber of rotor revolution was 50 rpm, the floating weight pressure was3 kg/cm², the kneading time was 5 minutes, and the kneading dischargetemperature was 145° C. Then, after the temperature of the above mixturewas observed to become 40° C., using a 14-inch roll, the above mixturewas kneaded with 1.5 parts by weight of “Sanceler PZ” (product name;manufactured by Sanshin Chemical Industry Co., Ltd.) as a vulcanizationpromoting assistant, 1.5 parts by weight of “Sanceler TT” (product name;manufactured by Sanshin Chemical Industry Co., Ltd.) as a vulcanizationpromoting assistant, 0.5 part by weight of “Sanceler M” (product name;manufactured by Sanshin Chemical Industry Co., Ltd.) as a vulcanizationpromoting assistant, and 0.75 part by weight of sulfur as a vulcanizingagent. Kneading conditions were such that the roll temperature was frontroll/rear roll=65° C./50° C., the number of roll revolution was frontroll/rear roll=13 rpm/11.5 rpm, the interval between rolls was 5 mm, andthe kneading time was 8 minutes, thereby performing sheeting. Then, thismixture was subjected to vulcanization at 170° C. for 10 minutes using apress molding machine, to thereby prepare a rubber sheet with athickness of 2 mm, and then properties were measured. Results of variousmeasurements are shown in Table 5.

Example 45

The same operation was performed as in Example 44, except that the4-methyl-1-pentene/α-olefin copolymer obtained in Example 1 was used inan amount of 30 parts by weight, thereby preparing a rubber sheet with athickness of 2 mm, and properties were measured. Results of variousmeasurements are shown in Table 5.

Example 46

The same operation was performed as in Example 44, except that the4-methyl-1-pentene/α-olefin copolymer obtained in Example 4 was used inan amount of 15 parts by weight, thereby preparing a rubber sheet with athickness of 2 mm, and properties were measured. Results of variousmeasurements are shown in Table 5.

Example 47

The same operation was performed as in Example 44, except that the4-methyl-1-pentene/α-olefin copolymer obtained in Example 4 was used inan amount of 30 parts by weight, thereby preparing a rubber sheet with athickness of 2 mm, and properties were measured. Results of variousmeasurements are shown in Table 5.

Comparative Example 9

The same operation was performed as in Example 44, except that the4-methyl-1-pentene/α-olefin copolymer was not contained, therebypreparing a rubber sheet with a thickness of 2 mm, and properties weremeasured. Results of various measurements are shown in Table 5.

TABLE 5 Ex. 44 Ex. 45 Ex. 46 Ex. 47 Com. Ex. 9 Polymer (A) Example 1 1530 Example 4 15 30 Thermoplastic resin (B) 3072EM 140 140 140 140 140Zinc oxide 5 5 5 5 5 Stearic acid 1 1 1 1 1 SEAST G116 80 80 80 80 80PW-380 47 47 47 47 47 EL % 700 680 700 680 720 TS MPa 18 13 16 14 19Shore hardness (immediately after) 54 52 54 53 55 Shore hardness (15 secafter) 44 40 43 43 46 Hardness meter type A A A A A ΔHS 10 12 11 10 9Temperature giving tan δ peak ° C. −42 −40 −39 −41 −41 tan δ peak value0.5 0.4 0.5 0.5 0.5 tan δ value (−15° C.) 0.22 0.34 0.18 0.18 0.10 tan δvalue (10° C.) 0.12 0.14 0.18 0.28 0.12 Ball drop resilience ratio (25°C.) % 24 17 24 24 30

Polymerization Example (AA-1)

Into a SUS autoclave with an agitating element having a volume of 1.5 Lthat had been sufficiently purged with nitrogen, at 23° C., 750 mL of4-methyl-1-pentene was introduced. Into this autoclave, 0.75 mL of atoluene solution of 1.0 mmol/mL of triisobutylaluminum (TIBAl) wasintroduced, and the agitator was operated. Then, the autoclave washeated till the temperature of the mixture became 30° C., andpressurization using propylene was performed such that the totalpressure became 0.74 MPaG. Then, 0.34 mL of a previously-preparedtoluene solution containing 1 mmol in terms of Al of methylaluminoxaneand 0.005 mmol of diphenylmethylene (1-ethyl-3-t-butyl-cyclopentadienyl)(2,7-di-t-butyl-fluorenyl)zirconiumdichloride was injected usingnitrogen into the autoclave, thereby initiating polymerization. For thefollowing 60 minutes, temperature of the autoclave was controlled suchthat the temperature of the mixture was 60° C. At 60 minutes past theinitiation of the polymerization, 5 mL of methanol was injected usingnitrogen into the autoclave, thereby terminating the polymerization anddepressurizing the autoclave to atmospheric pressure. Into the reactionsolution, acetone was poured with stirring. The resultantsolvent-containing rubber polymer was dried at 130° C. under reducedpressure for 12 hours.

The resultant polymer weighed 56.3 g, and the content of propylene inthe polymer was 40.4 wt %. With regard to the polymer, Tm was notobserved; the intrinsic viscosity [η] was 1.5 dL/g; the molecular weightdistribution obtained by GPC was such that Mw was 287000, Mn was 144000,and Mw/Mn was 2.0; and ΔHS was 14. Properties of the resultant polymerare shown in Table 6.

Polymerization Example (AA-2)

Into a SUS autoclave with an agitating element having a volume of 1.5 Lthat had been sufficiently purged with nitrogen, at 23° C., 750 mL of4-methyl-1-pentene was introduced. Into this autoclave, 0.75 mL of atoluene solution of 1.0 mmol/mL of triisobutylaluminum (TIBAl) wasintroduced, and the agitator was operated. Then, the autoclave washeated till the temperature of the mixture became 30° C., andpressurization using propylene was performed such that the totalpressure became 0.68 MPaG. Then, 0.34 mL of a previously-preparedtoluene solution containing 1 mmol in terms of Al of methylaluminoxaneand 0.005 mmol of diphenylmethylene(1-methyl-3-t-butyl-cyclopentadienyl)(2,7-di-t-butyl-fluorenyl)zirconiumdichloride was injected usingnitrogen into the autoclave, thereby initiating polymerization. For thefollowing 60 minutes, temperature of the autoclave was controlled suchthat the temperature of the mixture was 60° C. At 60 minutes past theinitiation of the polymerization, 5 mL of methanol was injected usingnitrogen into the autoclave, thereby terminating the polymerization anddepressurizing the autoclave to atmospheric pressure. Into the reactionsolution, acetone was poured with stirring. The resultantsolvent-containing rubber polymer was dried at 130° C. under reducedpressure for 12 hours.

The resultant polymer weighed 45.9 g, and the content of4-methyl-1-pentene in the polymer was 47.4 wt %. With regard to thepolymer, Tm was not observed; the intrinsic viscosity [η] was 1.47 dL/g;the molecular weight distribution obtained by GPC was such that Mw was310000, Mn was 155000, and Mw/Mn was 2.0; and ΔHS was 24. Properties ofthe resultant polymer are shown in Table 6.

Polymerization Example (AA-3)

Polymerization was performed in the same manner as in PolymerizationExample AA-2, except that the pressurization using propylene wasperformed such that the total pressure in the polymerization containerwas 0.35 MPaG.

The resultant polymer weighed 46.9 g, and the content of4-methyl-1-pentene in the polymer was 64.0 wt %. With regard to thepolymer, Tm was not observed; the intrinsic viscosity [η] was 1.41 dL/g;the molecular weight distribution obtained by GPC was such that Mw was285000, Mn was 143000, and Mw/Mn was 2.0; and ΔHS was 38. Properties ofthe resultant polymer are shown in Table 6.

Polymerization Example (AA-4)

Polymerization was performed in the same manner as in PolymerizationExample AA-2, except that the pressurization using propylene wasperformed such that the total pressure in the polymerization containerwas 0.15 MPaG.

The resultant polymer weighed 46.9 g, and the content of4-methyl-1-pentene in the polymer was 76.6 wt %. With regard to thepolymer, Tm was not observed; the intrinsic viscosity [η] was 1.44 dL/g;the molecular weight distribution obtained by GPC was such that Mw was295000, Mn was 142000, and Mw/Mn was 2.09; and ΔHS was 40. Properties ofthe resultant polymer are shown in Table 6.

Polymerization Example (AA-5)

Polymerization was performed in the same manner as in PolymerizationExample AA-2, except that the pressurization using propylene wasperformed such that the total pressure in the polymerization containerwas 0.15 MPaG, and the polymerization temperature was 60° C.

The resultant polymer weighed 24.0 g, and the content of4-methyl-1-pentene in the polymer was 83.0 wt %. With regard to thepolymer, Tm was not observed; the intrinsic viscosity [η] was 1.31 dL/g;the molecular weight distribution obtained by GPC was such that Mw was257000, Mn was 124000, and Mw/Mn was 2.08; and ΔHS was 24. Properties ofthe resultant polymer are shown in Table 6.

TABLE 6 Polymerization Example AA-1 AA-2 AA-3 AA-4 AA-5 Composition 4MP1wt % 40 47 64 77 83 α-olefin content(1) wt % 60 53 36 23 17 α-olefintype propylene propylene propylene propylene propylene Molecular [η]dL/g 1.5 1.5 1.4 1.4 1.3 weight Mw/Mn 2.0 2.0 2.0 2.1 2.1 Mw 287000310000 285000 295000 257000 Heat Tm ° C. Not Not Not Not Not resistanceObserved Observed Observed Observed observed Flexibility Shore hardness(immediately after) 40 52 72 94 96 Shore hardness(15 sec after) 26 28 3454 72 Hardness meter type A A A A A ΔHS 14 24 38 40 24 StressTemperature giving tan δ peak ° C. 6 11 19 25 26 Absorption tan δ peakvalue 3.5 3.2 3.4 2.8 2.5

[Crystalline Olefin Resin (BB-1)]

A commercially-available polypropylene (F107P, manufactured by PrimePolymer Co., Ltd.) was used. Properties of the polymer are shown inTable 7.

[Crystalline Olefin Resin (BB-2)]

A commercially-available polypropylene (F327, manufactured by PrimePolymer Co., Ltd.) was used. Properties of the polymer are shown inTable 7.

[Crystalline Olefin Resin (BB-3)]

Into a glass autoclave having a volume of 500 mL that had beensufficiently purged with nitrogen, 250 mL of toluene was introduced, 150L/h of propylene was flown, and were kept at 25° C. for 20 minutes. Onthe other hand, into a side-arm flask having a volume of 30 mL that hadbeen sufficiently purged with nitrogen, a magnetic stirrer was placed,and thereto, 5.00 mmol of a toluene solution of methylaluminoxane(Al=1.53 mol/L), and then 5.0 pmol of a toluene solution ofdibenzylmethylene (cyclopentadienyl)(3,6-di-tert-butylfluorenyl)zirconiumdichloride were added, and themixture was stirred for 20 minutes. This solution was added to thetoluene charged in the glass autoclave into which propylene had beenflown, thereby initiating polymerization. A propylene gas in an amountof 150 L/h was continuously fed, and under ordinary pressure,polymerization was performed at 25° C. for 45 minutes. Then, a slightamount of methanol was added to terminate the polymerization. Thepolymer solution was added to a large excess of methanol to precipitatethe polymer. The precipitated polymer was dried under reduced pressureat 80° C. for 12 hours. As a result, 2.38 g of the polymer was obtained.Properties of the resultant polymer are shown in Table 7.

[Crystalline Olefin Resin (BB-4)]

A commercially-available polypropylene (B241, manufactured by PrimePolymer Co., Ltd.) was used. Properties of the polymer are shown inTable 7.

[Crystalline Olefin Resin (BB-5)]

A commercially-available polypropylene (E-200GP, manufactured by PrimePolymer Co., Ltd.) was used. Properties of the polymer are shown inTable 7.

TABLE 7 Crystalline olefin resin (BB) BB-1 BB-2 BB-3 BB-4 BB-5 PP PP PPPP PP MFR g/10 min 7 7 6 0.5 2 Density g/cm³ 902 896 882 910 902 Meltingpoint (Tm) ° C. 160 140 155 160 160

[α-Olefin Copolymer (CC-1)]

Into a 1000 mL polymerization apparatus that had been sufficientlypurged with nitrogen, 1834 mL of a dried hexane, 1144 g of 1-octene, andtriisobutylaluminum (1.0 mmol) were introduced at ordinary temperature.Then, the polymerization apparatus was heated till the temperature ofthe mixture became 80° C., and the pressure inside the system wascontrolled to be 0.75 MPa using ethylene. Then, a toluene solution inwhich 0.003 mmol of bis(p-tolyl)methylene(cyclopentadienyl)(1,1,4,4,7,7,10,10-octamethyl-1,2,3,4,7,8,9,10-octahydrodibenz(b,h)-fluorenyl)zirconiumdichloridehad been contacted with 0.15 mmol in terms of aluminum ofmethylaluminoxane (manufactured by Tosoh Finechem Corporation) was addedinto the polymerization apparatus. With the temperature of the mixtureat 80° C., and with the pressure inside the system kept at 0.75 MPausing ethylene, polymerization was performed for 60 minutes. Then, 20 mLof methanol was added to terminate the polymerization. Afterdepressurization, in 4 L of methanol, the polymer was precipitated fromthe polymer solution, and the polymer was dried under vacuum at 130° C.for 12 hours. The resultant polymer weighed 75.0 g. Properties of theresultant polymer are shown in Table 8.

[α-Olefin Copolymer (CC-2)

Into a 4000 mL polymerization apparatus that had been sufficientlypurged with nitrogen, 1834 mL of a dried hexane and triisobutylaluminum(1.0 mmol) were introduced at ordinary temperature. Then, thepolymerization apparatus was heated till the temperature of the mixturebecame 80° C., and the pressure was increased so as to be 0.35 MPa usingpropylene, and then the pressure inside the system was controlled to be0.75 MPa using ethylene. Then, a toluene solution in which 0.00015 mmolof bis(p-tolyl)methylene(cyclopentadienyl) (1,1,4,4,7,7,10,10-octamethyl-1,2,3,4,7,8,9,10-octahydrodibenz(b,h)-fluorenyl)zirconiumdichloridehad been contacted with 0.075 mmol in terms of aluminum ofmethylaluminoxane (manufactured by Tosoh Finechem Corporation) was addedinto the polymerization apparatus. With the temperature of the mixtureat 80° C., and with the pressure inside the system kept at 0.75 MPausing ethylene, polymerization was performed for 60 minutes. Then, 20 mLof methanol was added to terminate the polymerization. Afterdepressurization, in 4 L of methanol, the polymer was precipitated fromthe polymer solution, and the polymer was dried under vacuum at 130° C.for 12 hours. The resultant polymer weighed 89.2 g. Properties of theresultant polymer are shown in Table 8.

[α-Olefin Copolymer (CC-3)]

Into a 4000 mL polymerization apparatus that had been sufficientlypurged with nitrogen, 1834 mL of a dried hexane, 90 g of 1-butene, andtriisobutylaluminum (1.0 mmol) were introduced at ordinary temperature.Then, the polymerization apparatus was heated till the temperature ofthe mixture became 80° C., and the pressure inside the system wascontrolled to be 0.75 MPa using ethylene. Then, a toluene solution inwhich 0.00015 mmol of bis(p-tolyl)methylene(cyclopentadienyl)(1,1,4,4,7,7,10,10-octamethyl-1,2,3,4,7,8,9,10-octahydrodibenz(b,h)-fluorenyl)zirconiumdichloridehad been contacted with 0.075 mmol in terms of aluminum ofmethylaluminoxane (manufactured by Tosoh Finechem Corporation) was addedinto the polymerization apparatus. With the temperature of the mixtureat 80° C., and with the pressure inside the system kept at 0.75 MPausing ethylene, polymerization was performed for 60 minutes. Then, 20 mLof methanol was added to terminate the polymerization. Afterdepressurization, in 4 L of methanol, the polymer was precipitated fromthe polymer solution, and the polymer was dried under vacuum at 130° C.for 12 hours. The resultant polymer weighed 49.0 g. Properties of theresultant polymer are shown in Table 8.

[α-Olefin Copolymer (CC-4)]

Into a 4000 mL polymerization apparatus that had been sufficientlypurged with nitrogen, 1834 mL of a dried hexane, 120 g of 1-butene, andtriisobutylaluminum (1.0 mmol) were introduced at ordinary temperature.Then, the polymerization apparatus was heated till the temperature ofthe mixture became 60° C., and the pressure was increased so as to be0.56 MPa using propylene, and then the pressure inside the system wascontrolled to be 0.75 MPa using ethylene. Then, a toluene solution inwhich 0.001 mmol of diphenylmethylene(3-tert-butyl-5-methyl-cyclopentadienyl)(2,7-di-tert-butyl-fluorenyl)zirconiumdichloride had been contacted with0.3 mmol in terms of aluminum of methylaluminoxane (manufactured byTosoh Finechem Corporation) was added into the polymerization apparatus.With the temperature of the mixture at 60° C., and with the pressureinside the system kept at 0.75 MPa using ethylene, polymerization wasperformed for 20 minutes. Then, 20 mL of methanol was added to terminatethe polymerization. After depressurization, in 4 L of methanol, thepolymer was precipitated from the polymer solution, and the polymer wasdried under vacuum at 130° C. for 12 hours. The resultant polymerweighed 102.5 g. Properties of the resultant polymer are shown in Table8.

[α-Olefin Copolymer (CC-5)]

Into a 4000 mL polymerization apparatus that had been sufficientlypurged with nitrogen, 1834 mL of a dried hexane, 110 g of 1-butene, andtriisobutylaluminum (1.0 mmol) were introduced at ordinary temperature.Then, the polymerization apparatus was heated till the temperature ofthe mixture became 55° C., and the pressure was increased so as to be0.56 MPa using propylene, and then the pressure inside the system wascontrolled to be 0.75 MPa using ethylene. Then, a toluene solution inwhich 0.001 mmol of diphenylmethylene(3-tert-butyl-5-methyl-cyclopentadienyl)(2,7-di-tert-butyl-fluorenyl)zirconiumdichloride had been contacted with0.3 mmol in terms of aluminum of methylaluminoxane (manufactured byTosoh Finechem Corporation) was added into the polymerization apparatus.With the temperature of the mixture at 55° C., and with the pressureinside the system kept at 0.75 MPa using ethylene, polymerization wasperformed for 25 minutes. Then, 20 mL of methanol was added to terminatethe polymerization. After depressurization, in 4 L of methanol, thepolymer was precipitated from the polymer solution, and the polymer wasdried under vacuum at 130° C. for 12 hours. The resultant polymerweighed 120.2 g. Properties of the resultant polymer are shown in Table8.

[α-Olefin Copolymer (CC-6)]

Into a 2000 mL polymerization apparatus that had been sufficientlypurged with nitrogen, 775 mL of a dried hexane, 135 g of 1-butene, andtriisobutylaluminum (1.0 mmol) were introduced at ordinary temperature.Then, the polymerization apparatus was heated till the temperature ofthe mixture became 50° C., and the pressure was increased so as to be0.7 MPa using propylene. Then, a toluene solution in which 0.002 mmol ofdimethylmethylene (3-tert-butyl-5-methylcyclopentadienyl) fluorenylzirconiumdichloride had been contacted with 0.6 mmol in terms ofaluminum of methylaluminoxane (manufactured by Tosoh FinechemCorporation) was added into the polymerization apparatus. With thetemperature of the mixture at 50° C., and with the propylene pressurekept at 0.7 MPa, polymerization was performed for 30 minutes. Then, 20mL of methanol was added to terminate the polymerization. Afterdepressurization, in 2 L of methanol, the polymer was precipitated fromthe polymer solution, and the polymer was dried under vacuum at 130° C.for 12 hours. The resultant polymer weighed 45.3 g. Properties of theresultant polymer are shown in Table 8.

[α-Olefin Copolymer (CC-7)]

Into a 2000 mL polymerization apparatus that had been sufficientlypurged with nitrogen, 775 mL of a dried hexane, 300 g of 1-butene, andtriethylaluminum (1.0 mmol) were introduced at ordinary temperature.Then, 240 NmL of a hydrogen gas was introduced, and the polymerizationapparatus was heated till the temperature of the mixture became 60° C.,and then the pressure was increased so as to be 0.7 MPa using propylene.Then, a toluene solution of 0.013 mmol of a prepared solid titaniumcatalyst was added into the polymerization apparatus. With thetemperature of the mixture at 50° C., and with the propylene pressurekept at 0.7 MPa, polymerization was performed for 30 minutes. Then, 20mL of methanol was added to terminate the polymerization. Afterdepressurization, in 2 L of methanol, the polymer was precipitated fromthe polymer solution, and the polymer was dried under vacuum at 130° C.for 12 hours. The resultant polymer weighed 65.3 g. Properties of theresultant polymer are shown in Table 8.

TABLE 8 Olefin copolymer (CC) Polymerization Example CC-1 CC-2 CC-3 CC-4CC-5 CC-6 CC-7 α-olefin content (1) wt % 59 74 71 69 66 71 80 α-olefintype (1) ethylene ethylene ethylene propylene propylene propylene buteneα-olefin content (2) wt % 41 26 29 18 14 29 20 α-olefin type (2) octenepropylene butene butene butene butene propylene α-olefin content (3) wt% 13 20 α-olefin type (3) ethylene ethylene MFR g/10 min  1 0.8  4  7  1 7  4 Density g/cm³ 870  869 864  857  858  890  887  Melting point (Tm)° C. 38 42 50 50 60 70 75

Example Y-1

70 parts by weight of the 4-methyl-1-pentene copolymer (AA-1), 20 partsby weight of the crystalline olefin resin (BB-4), and 10 parts by weightof the olefin copolymer (CC-3) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-2

60 parts by weight of the 4-methyl-1-pentene copolymer (AA-1), 20 partsby weight of the crystalline olefin resin (BB-4), and 20 parts by weightof the olefin copolymer (CC-3) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-3

70 parts by weight of the 4-methyl-1-pentene copolymer (AA-1), 10 partsby weight of the crystalline olefin resin (BB-5), and 20 parts by weightof the olefin copolymer (CC-6) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-4

70 parts by weight of the 4-methyl-1-pentene copolymer (AA-1), 20 partsby weight of the crystalline olefin resin (BB-5), and 10 parts by weightof the olefin copolymer (CC-6) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-5

70 parts by weight of the 4-methyl-1-pentene copolymer (AA-1), 20 partsby weight of the crystalline olefin resin (BB-5), and 10 parts by weightof the olefin copolymer (CC-7) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-6

70 parts by weight of the 4-methyl-1-pentene copolymer (AA-2), 20 partsby weight of the crystalline olefin resin (BB-1), and 10 parts by weightof the olefin copolymer (CC-3) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-7

80 parts by weight of the 4-methyl-1-pentene copolymer (AA-3), 4 partsby weight of the crystalline olefin resin (BB-2), and 16 parts by weightof the olefin copolymer (CC-4) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-8

60 parts by weight of the 4-methyl-1-pentene copolymer (AA-6), 8 partsby weight of the crystalline olefin resin (BB-2), and 32 parts by weightof the olefin copolymer (CC-4) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-9

80 parts by weight of the 4-methyl-1-pentene copolymer (AA-4), 3 partsby weight of the crystalline olefin resin (BB-3), and 17 parts by weightof the olefin copolymer (CC-5) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-10

60 parts by weight of the 4-methyl-1-pentene copolymer (AA-4), 6 partsby weight of the crystalline olefin resin (BB-3), and 34 parts by weightof the olefin copolymer (CC-5) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Example Y-11

60 parts by weight of the 4-methyl-1-pentene copolymer (AA-4), 6 partsby weight of the crystalline olefin resin (BB-3), and 34 parts by weightof the olefin copolymer (CC-5) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that improved strength wasobtained, and it is clear from the ball drop resilience ratio thatimproved stress absorption was obtained.

Reference Example y-1

10 parts by weight of the 4-methyl-1-pentene copolymer (AA-2), 80 partsby weight of the crystalline olefin resin (BB-2), and 10 parts by weightof the olefin copolymer (CC-1) were blended with one another. Further,100 parts by weight of the composition was blended with 1000 ppm ofIrganox 1010, a hindered phenol-based antioxidant, 1000 ppm of Irgafos168, a phosphorus-based processing heat stabilizer, each of which ismanufactured by Ciba Japan K.K., and 500 ppm of calcium stearatemanufactured by NOF Corporation. Then, these were melt kneaded using aLabo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

Comparative Example y-2

70 parts by weight of the crystalline olefin resin (BB-1) and 30 partsby weight of the olefin copolymer (CC-1) were blended with one another.Further, 100 parts by weight of the composition was blended with 1000ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000 ppm ofIrgafos 168, a phosphorus-based processing heat stabilizer, each ofwhich is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

It is clear from the mechanical properties that the strength isinferior, and it is clear from the ball drop resilience ratio that thestress absorption is inferior.

Reference Example y-3

40 parts by weight of the 4-methyl-1-pentene copolymer (AA-1) and 60parts by weight of the crystalline olefin resin (BB-1) were blended withone another. Further, 100 parts by weight of the composition was blendedwith 1000 ppm of Irganox 1010, a hindered phenol-based antioxidant, 1000ppm of Irgafos 168, a phosphorus-based processing heat stabilizer, eachof which is manufactured by Ciba Japan K.K., and 500 ppm of calciumstearate manufactured by NOF Corporation. Then, these were melt kneadedusing a Labo Plastomill (a biaxial batch type melt kneading apparatus)manufactured by Toyo Seiki Seisaku-Sho Ltd., with the temperature set at200° C., with the resins charged in an amount of 40 g (apparatus batchvolume=60 cm³), at 50 rpm, for 5 minutes. Then, the mixture wascollected and cooled using a cooling press set at 20° C., to therebyform a sheet. The sheet was cut so as to have an appropriate size,thereby preparing a specimen for measurement. Furthermore, using thespecimen, a press sheet was prepared and properties were measured.Results of various measurements are shown in Table 9.

TABLE 9 Ex. Y-1 Ex. Y-2 Ex. Y-3 Ex. Y-4 Ex. Y-5 Ex. Y-64-methyl-1-pentene copolymer (A) AA-1 AA-1 AA-1 AA-1 AA-1 AA-2Crystalline olefin resin (B) BB-4 BB-4 BB-5 BB-5 BB-5 BB-1 Olefincopolymer (C) CC-3 CC-3 CC-6 CC-6 CC-7 CC-3 (A)/(B)/(C) compositionalratio (wt %) 70/20/10 60/20/20 70/10/20 70/20/10 70/20/10 70/20/10 EL %848 990 861 922 643 874 TS MPa 11 14 22 35 12 17 YM MPa 11 11 13 57 616.9 Shore hardness (immediately after) 75 76 80 94 83 76 Shore hardness(15 sec after) 59 66 69 84 72 63 Hardness meter type A A A A A A ΔHS 1610 11 10 11 13 Temperature giving tan δ peak ° C. 8 8 9 9 8 12 tan δpeak value 1.1 0.9 1.0 0.6 0.9 1.0 Ball drop resilience ratio (25° C.) %7 8 8 10 10 6 Ex. Y-7 Ex. Y-8 Ex. Y-9 Ex. Y-10 Ex. Y-114-methyl-1-pentene copolymer (A) AA-3 AA-4 AA-4 AA-4 AA-4 Crystallineolefin resin (B) BB-2 BB-2 BB-3 BB-3 BB-3 Olefin copolymer (C) CC-4 CC-4CC-5 CC-5 CC-5 (A)/(B)/(C) compositional ratio (wt %) 80/4/16 60/8/3280/3/17 60/6/34 60/6/34 EL % 687 778 640 732 614 TS MPa 9 14 7 11 22 YMMPa 3 5 3 7 33 Shore hardness (immediately after) 66 64 68 75 71 Shorehardness (15 sec after) 37 44 41 44 52 Hardness meter type A A A A A ΔHS29 20 27 31 19 Temperature giving tan δ peak ° C. 14 16 15 14 23 tan δpeak value 1.9 1.4 1.8 1.1 1.3 Ball drop resilience ratio (25° C.) % 612 15 10 25 Ref. Ref. Ref. Ex. y-1 Ex. y-2 Ex. y-3 4-methyl-1-pentenecopolymer (A) AA-2 AA-1 Crystalline olefin resin (B) BB-2 BB-1 BB-1Olefin copolymer (C) CC-1 CC-1 (A)/(B)/(C) compositional ratio (wt %)10/80/10 0/70/30 40/60/0 EL % 375 274 535 TS MPa 24 16 30 YM MPa 795 686343 Shore A hardness (immediately after) 54 56 66 Shore A hardness (15sec after) 49 53 56 Hardness meter type D D D ΔHS 5 3 10 Temperaturegiving tan δ peak ° C. −23 −20 5.2 tan δ peak value 0.1 0.1 0.3 Balldrop resilience ratio (25° C.) % 32 48 25

1. A 4-methyl-1-pentene/α-olefin copolymer composition (X21) comprising:50 to 95 parts by weight of the 4-methyl-1-pentene/α-olefin copolymer(A2) comprising 50 to 75 mol % of a structural unit (i) derived from4-methyl-1-pentene, 50 to 25 mol % of a structural unit (ii) derivedfrom at least one kind of α-olefin selected from ethylene and propyleneand 0 to 5 mol % of a structural unit (iii) derived from anon-conjugated polyene, provided that the total of the structural units(i), (ii), and (iii) is 100 mol %, wherein the copolymer (A2) satisfiesthe following requirements (a) to (d) and (e1): (a): the intrinsicviscosity [η], as measured in decalin at 135° C., is 0.01 to 1.7 dL/g,(b): the ratio (Mw/Mn) of a weight-average molecular weight (Mw) to anumber-average molecular weight (Mn), as measured by gel permeationchromatography (GPC), is 1.0 to 3.5, (c): the tensile modulus (YM) is0.1 to 1000 MPa, (d): the melting point [Tm], as measured bydifferential scanning calorimetry (DSC), is lower than 110° C. or notobserved, and (e1): the change ΔHS in Shore A hardness, defined by thefollowing equation, is 15 to 50, Shore A hardness being measured using apress sheet thereof having a thickness of 3 mm in accordance with JISK6253, withΔHS=Shore A hardness immediately after the starting of indentercontact−Shore A hardness 15 seconds after the starting of indentercontact; and 5 to 50 parts by weight of a thermoplastic resin (B) otherthan the 4-methyl-1-pentene/α-olefin copolymer (A), provided that thetotal of the copolymer (A) and the thermoplastic resin (B) is 100 partsby weight, wherein the composition satisfies the following requirement(e2): (e2): the change ΔHS in Shore A hardness, defined by the followingequation, is 10 to 50, Shore A hardness being measured using a presssheet thereof having a thickness of 3 mm in accordance with JIS K6253;or the change ΔHS in Shore D hardness, defined by the followingequation, is 5 to 50, Shore D hardness being measured using a presssheet thereof having a thickness of 3 mm in accordance with JIS K6253,withΔHS=Shore A hardness or Shore D hardness immediately after the startingof indenter contact−Shore A hardness or Shore D hardness 15 secondsafter the starting of indenter contact.
 2. A 4-methyl-1-pentene/α-olefincopolymer composition (X22) comprising: 5 to 49 parts by weight of the4-methyl-1-pentene/α-olefin copolymer (A2) comprising 50 to 75 mol % ofa structural unit (i) derived from 4-methyl-1-pentene, 50 to 25 mol % ofa structural unit (ii) derived from at least one kind of α-olefinselected from ethylene and propylene and 0 to 5 mol % of a structuralunit (iii) derived from a non-conjugated polyene, provided that thetotal of the structural units (i), (ii), and (iii) is 100 mol %, whereinthe copolymer (A2) satisfies the following requirements (a) to (d) and(e1): (a): the intrinsic viscosity [η], as measured in decalin at 135°C., is 0.01 to 1.7 dL/g, (b): the ratio (Mw/Mn) of a weight-averagemolecular weight (Mw) to a number-average molecular weight (Mn), asmeasured by gel permeation chromatography (GPC), is 1.0 to 3.5, (c): thetensile modulus (YM) is 0.1 to 1000 MPa, (d): the melting point [Tm], asmeasured by differential scanning calorimetry (DSC), is lower than 110°C. or not observed, and (e1): the change ΔHS in Shore A hardness,defined by the following equation, is 15 to 50, Shore A hardness beingmeasured using a press sheet thereof having a thickness of 3 mm inaccordance with JIS K6253, withΔHS=Shore A hardness immediately after the starting of indentercontact−Shore A hardness 15 seconds after the starting of indentercontact; and 51 to 95 parts by weight of a thermoplastic resin (B) otherthan the 4-methyl-1-pentene/α-olefin copolymer (A), provided that thetotal of the copolymer (A) and the thermoplastic resin (B) is 100 partsby weight.
 3. An article comprising the 4-methyl-1-pentene/α-olefincopolymer composition according to claim
 1. 4. An article comprising the4-methyl-1-pentene/α-olefin copolymer composition according to claim 2.